    [From the U.S. Government Printing Office, www.gpo.gov]

                                                                          1A

                                                                               OCT

                                                   INVENTORY OF HEAVY METALS DATA:
                                                       LOUISIANA COASTAL ZONE

                                   COASTAL ZONE
                               INFORMATION CENTER

                                                            Submitted by

                                                         Marty E. Tittlebaum
                                                   Department of Civil Engineering
                                                     Louisiana State University
            CN-                                         Baton Rouge, LA 70803

                                                            Submitted to

                                                    John deMond, Project Manager
                                              Louisiana Department of Natural Resources

                 TD
                 196
                 M4
                 T5

                                                 TABLE OF CONTENTS

                                                                                          Page

                     1.   INTRODUCTION  . . . . . . . . . . . . . . . . . . . . . . .        1

                     2.   DATA COLLECTION   . . . . . . . . . . . . . . . . . . . . .        2

                     3.   ASSESSMENT OF DATA  . . . . . . . . . . . . . . . . . . . .        3

                     4.   RECOMMENDATIONS   . . . . . . . . . . . . . . . . . . . . . .     15

                     5.   REFERENCES  . . . . . . . . . . . . . . . . . . . . . . . .       23

                     6.   BIBLIOGRAPHY  . . . . . . . . . . . . . . . . . . . . . . .       27

                     7.   APPENDICES

                               A     1:250,000 Location Maps
                                     (separate document six total)

                               B     Data Printout, Software and
                                     Instructions (separate document)

                               C     Excursions from USGS Sediment
                                     Alert Level and Statewide
                                     Order 29-B Limitations

                                                1. INTRODUCTION

                         During the past five years, there have been numerous, independent

                     reports of heavy metal contamination in Louisiana's aquatic ecosystems.

                     The Louisiana Department of Environmental Quality has most recently

                     investigated metal contamination in sediments of Bayou Trepaigner,

                     Calcasieu River, Caddo Lake and Devil's Swamp. Louisiana State

                     University researchers (Tittlebaum. and White, 1983) found heavy metal

                     enrichment in a Baton Rouge urban lake and two waterways in New Orleans.

                     In a 1984 feasibility study, the U.S. Army Ccrps of Engineers suggests

                     that heavy metals from the Mississippi River and its sediments may serve

                     as possible contaminants for the hydrologic basins receiving fresh-water

                     diverted from the Mississippi for the purposes of retarding salt water

                     intrusion into delta plain estuaries and marshes. In a 1981 Environ-

                     mental Impact Statement, the U.S. Coast Guard recommends that the State

                     consider constructing a bridge on a stretch of U.S. Highway 90 near

                     Morgan City, rather than a ground-level highway, to prevent the release

                     of mercury from sediments disturbed by dredging operations.

                          Toxic heavy metals such as zinc, cadmium, lead, mercury and arsenic

                     are potential health hazards in at least a few known locations in

                     Louisiana. Heavy metals tend to accumulate in Louisiana's highly

                     organic bottom sediments, from which they can be remobilized and move up

                     to biologic food chain, affecting valuable aquatic resources as well as

                     human health.

                          The Office of Conservation of the Louisiana Department of Natural

                     Resources (DNR) has enacted new regulations governing oil field waste

                     disposal in wetland environments. Disposal techniques include

                     landfarming which is intended to dispose of trace metal-bearing muds and

                                                                                               2

                      fluids without increasing the level of these metals above acceptable

                      standards. This approach will be reviewed on a case-by-case basis by

                      the DNR Coastal Management Division (CMD) for every oil field waste

                      disposal pit in the coastal zone. To properly assess each project, CMD

                      must have a significant amount of widely varying information including

                      background levels of trace metals in coastal ecosystems.

                           This report provides an inventory of existing sediment trace metal

                      data in a format that enables CMD coastal resource analysts to retrieve

                      and use it. It also identifies data deficiencies which may be the basis

                      for subsequent joint studies by CMD and the Office of Conservation to

                      remedy data gaps and increase the understanding of trace-metal mobility

                      in coastal environments.

                                                 2. DATA COLLECTION

                           The primary objective of this study is to compile an inventory of

                      heavy metals data for Louisiana coastal sediments which can be obtained

                      from published and unpublished sources. It is not the intent of this

                      project to investigate the severity of metal contamination in a

                      detailed, site specific manner. This would be especially difficult

                      without compiling data describing natural background levels of heavy

                      metals in Louisiana sediments. Rather, the intent is to compile data in

                      a format which will provide regulatory personnel within CMD with all

                      available sediment data relating to heavy metals for use in permit pro-

                      cessing.  The compilation of data includes the following heavy metals:

                                Aluminum             Cobalt                Nickel
                                Arsenic              Copper                Selenium
                                Barium               Iron                  Silver
                                Beryllium            Lead                  Vanadium
                                Cadmium              Manganese             Zinc
                                Chromium             Mercury

                                                                                             3

                          During the data,collection phase of the project, the researchers

                     developed a listing of the sources of all data obtained and a set of

                     maps showing the locations of the sampling stations for which data was

                     reported.

                          The study area defined by this project included twenty-one parishes

                     located in the Louisiana coastal zone; generally south of Highway I-10

                     (see Appendix A). Data from Jefferson County, Texas, was also included

                     in the study. Listed below are the included parishes:

                               Ascension                      Orleans
                               Assumption                     Plaquemines
                               Calcasieu                      St. Bernard
                               Cameron                        St. Charles
                               Iberia                         St. James
                               Iberville                      St. John
                               Jefferson                      St. Martin
                               Jefferson  Co., TX             St. Mary
                               Jefferson Davis                St. Tammany
                               Lafayette                      Terrebonne
                               Lafourche                      Vermillion

                          The appropriate state agencies that were contacted for heavy metals

                     data include the Department of Wildlife and Fisheries, Department of

                     Transportation and Development, Department of Natural Resources., and

                     Department of Environmental Quality.

                          Also contacted were the following Federal agencies: U.S. Environ-

                     mental Protection Agency, Region 6; U.S. Environmental Protection

                     Agency, Office of Water Regulations, Washington, DC; U.S. Army Corps of

                     Engineers, New Orleans District; U.S. Army Corps of Engineers, Waterways

                     Experiment Station, Vicksburg, MS; U.S. Coast Guard; U.S. Geological

                     Survey, Baton Rouge; U.S. Department of Wildlife and Fisheries, Slidell,

                     LA; National Space Technology Lab, Bay St. Louis, MS; USGS, Minerals

                     Management Service, Metairie, LA.

                                                                                            4

                          The universities contacted for metals data were Louisiana State

                     University, Baton Rouge; University of New Orleans; Tulane University;

                     University of Southeast Louisiana; Southwestern Louisiana State

                     University; Nichols State University; Texas A & M; and University of

                     South Alabama.

                          Inquiries were made to laboratories, engineering firms, environ-

                     mental companies and groups in the New Orleans and Baton Rouge areas for

                     non-proprietary heavy metals data. Requests were made to chemical

                     companies and petroleum companies for non-proprietary metals data.

                     These companies include: Texaco Oil Co., Amoco Oil Co., Freeport

                     Chemical, Freeport MacMoran, Mobile Oil Co., Kaiser Aluminum, Exxon Oil

                     Co... and Shell Oil Co.

                          A literature survey was run at the Middleton Library of Louisiana

                     State University using NTIS (National Technical Information Service),

                     GEOREF, oceanic abstracts, environmental bibliography, aquatic science,

                     and fisheries abstracts data bases. A complete listing of all sources

                     contacted is included in the bibliography.

                                             3. ASSESSMENT OF DATA

                          Through the course of this study, a large amount of sediment heavy

                     metal data was identified and cataloged into a computer software package

                     which can be updated and used to recall the data in various forms. Data

                     retrieval can be performed by various categories including by parish, by

                     sample number, and by coordinates. Also, by listing coordinates, the

                     program will identify the three nearest sample site locations and

                     determine the distance to those sample sites.

                          The total number of sediment heavy metal sample sites identified is

                     395. Many of these sites had multiple sampling dates associated with

                                                                                           5

                     them, yielding a total of 708 sample sets. Each set has one or more

                     sediment metal concentrations for the previously listed metals.

                     Specific operating instructions and program listing are included in

                     Appendix B together with a printout of all data identified.

                          Assessment of this large data bank was limited to two specific

                     areas of interest: biological accumulation of metals by aquatic life

                     forms and a state-wide summary of findings. The summary of findings

                     includes the identification of excursions from USGS sediment levels and

                     state-wide order 29-B limitations (Appendix C).

                     A.   Biological Accumulation of Metals by Aquatic Life Forms

                          The presence of toxic contaminants in terrestial and aquatic food

                     chains has been a major cause of concern due to the potential chronic or

                     acute harmful effects on living organisms. Many chemicals are frequently

                     present in the environment in extremely low concentrations, often below

                     the levels readily detectable by chemical and physical analytical tech-

                     niques. Aquatic organisms can readily absorb metals from their sur-

                     roundings, and may accumulate levels that are greatly in excess of the

                     ambient concentrations in their environment. Table 1 indicates concen-

                     trations above ambient levels in aquatic species sampled in Vermillion

                     Parish.

                          It is the ability of aquatic species to regulate abnormal concen-

                     trations that determines tolerances, and is a critical factor in sur-

                     vival. However, there is an upper limit to the amount of metal which

                     can be excreted by animals, above which there is an accumulation in body

                     tissues.

                          The initial uptake of metals by aquatic organisms can be considered

                     in terms of three main processes: (1) from water through respiratory

                                                                                                6

                                Table 1. Concentrations above ambient levels in
                                          aquatic species sampled in Vermillion
                                          Parish (11).

                                Arsenic

                                   Clams                                 6-15x
                                   Fish                                  up to IN

                                Cadmium

                                   Zooplankton (microscopic animals)     6,000x
                                   Oysters                               2,150x
                                   Clams                                 30 - 2,260,000x

                                Chromium

                                   Oyster                                60,000
                                   Clams                                 200 to 1,050x

                                Lead

                                   Zooplankton                           197,000
                                   Oysters                               3,300
                                   Clams                                 5,300

                                Mercury

                                   Plankton (microscopic plants)         20 - 100
                                   Shrimp                                20 - 55
                                   Oysters                               500 - 2,800
                                   Clams                                 1,223
                                   Fish                                  250
                                   Insects                               8,310

                                Silver

                                   Oysters                               18,700
                                   Clams                                 2,300
                                   Fish                                  120

                                Zinc

                                   Zooplankton                           5,100
                                   Algae                                 64,000
                                   Oysters                               750,000
                                   Shrimp                                5,600
                                   Crabs                                 5,800
                                   Fish                                  16,300
                                   Marsh Grass                           880

                                                                                           7

                     surfaces (e.g., gills), (2) adsorption from water onto body surfaces,

                     and (3) from ingested food, particles, or water through the digestive

                     system.

                          In the case of photo- and chemoautotrophic organisms, metal uptake

                     occurs directly from solution, or for higher plants additionally via the

                     roots. For many metals, rates of absorption are directly proportional

                     to the levels of availability in the environment.

                          Metal uptake from dietary sources in comparison to direct

                     adsorption from solution is of fundamental importance with heterotrophic

                     aquatic organisms. Available evidence is limited but indicates that

                     food and particulates are more important sources of metals than water,

                     for large animals such as fish and lobster. Within polluted aquatic

                     environments dietary preferences or feeding habits are significant

                     because of metal enrichment in sediments, particulates and detritus.

                          Bioconcentration of a metal is a complex process dependent not only

                     on the chemical parameters of the medium, but also on the physical

                     structure, i.e., size, sex, age, lipid storage and metabolism of the

                     biota, as well as species and half life of the metal. Data shows that

                     once absorbed, some metals are retained for long periods before being

                     flushed out of the system.

                          Metals have been placed into four different classes according to

                     their bioconcentration factor (BCF):

                                     Class                           BCF

                               Non-Accumulative                     < 60

                               Slightly Accumulative               60 - 70

                               Moderately Accumulative            700 - 800

                               Highly Accumulative                  > 8000

                                                                                           8

                          Table 2 shows the BCF's and half lives for most of the metals

                     identified in the study. There is no appreciable bioaccumulation for

                     beryllium, chromium, nickel, selenium and silver; as the BFC's were less

                     than 400. Arsenic, cadmium, copper, lead, mercury and zinc show a high

                     degree of bioaccumulation.

                          Chronic low dose (sublethal) exposure to heavy metals can lead to

                     changes in the histology or morphology of the tissues in fish and

                     crustacean species. These changes are secondary effects due to inter-

                     ference with enzyme processes involved in food utilization.

                          Supression in growth, reproduction circulation and respiration are

                     noted after exposure to relatively low metal concentrations. Reproduc-

                     tion in many aquatic organisms is affected in the parts per billion

                     range for most aquatic toxic metal ions. Changes also occur in blood

                     chemistry, endocrinology and enzyme activity after uptake or sublethal

                     quantities of metals. The observed behavioral changes are the impair-

                     ment of feeding and learning processes, swimming, and response to

                     external stimuli.

                          Studies of the community structure (species richment, species

                     composition and abundance) or epibenthic seagrass fauna show a decrease

                     of 20 common species, mostly fish, which were correlated with the

                     concentration of contaminant metals (Cd, Cu, Pb, Mn and Zn) in the

                     sediments. It was also found that the frequencies of certain species,

                     mostly crustaceans, correlated with particle size distributions. Both

                     contaminant metals and sediment particle size have substantial

                     controlling effects on the community structure. Heavy metals show a

                     greater effect on fish than crustaceans. Opportunistic epibenthic

                     species avoid a contaminated area.

                                                                                                9

                      Table 2. BCF's and Biological Half-Lives for Inorganic Contaminants
                                (28).

                      Contaminant          BCF         Biological        Source of Information
                                                       Half-Life

                      Arsenic           0-450         10-60 days         Waldichuk (1974; Woolson
                                                                         et al. (1976); Gidding &
                                                                         Eddleman (1977); U.S.
                                                                         EPA (1979

                      Beryllium         5-150         37-53 days         U.S. EPA (1979)

                      Cadmium           3-182,000     10-30 years        Waldichuk (1974; U.S.
                                                                         EPA (1979; Piotrowski &
                                                                         Coleman (1980); Friberg
                                                                         et al. (1974)

                      Chromium          1-152         616 days           U.S. EPA (1979
                      (trivalent)

                      Cooper            0-35,000      very short         Waldichuk (1974); Weber
                                                                         (1977); U.S. EPA (1979)

                      Lead             42-100,000     10 years           Waldichuk (1974); U.S.
                                                                         EPA (1979)
                      Mercury
                      (inorganic)     129-33,800      40-70 days         Waldichuk (1974); Weber
                                                                         (1977); U.S. EPA (1979);
                                                                         Piotrowski and Coleman
                                                                         (1980)

                      Nickel          918-61          very short         U.S. EPA (1979)

                      Selenium          2-20          1-several days     U.S. EPA (1979)

                      Silver            0-368         15-52 days         U.S. EPA (1979)

                      Zinc              1-27,080      200-400 days       U.S. EPA (1979)

                      *BCF's reported are for both   freshwater and marine oranisms. Biological
                       half-life is the estimated time for excretion of 50% of the total
                       ingested metal from the biological system.

                                                                                           10

                          Several general characteristics of metal toxicity within aquatic

                    organisms can be expressed:

                          (1)  Metal ions and complexes exhibit a wide range of toxicity to

                               marine and freshwater organisms.

                          (2)  In fish, the rate of absorption of methyl mercury is faster

                               than that for inorganic mercury (bacteria are capable or

                               transforming inorganic mercury compounds into dimethyl and

                               methyl mercury), and the clearance rate is lower, with a net

                               result of high methyl mercury concentrations in the muscle

                               tissue.

                          (3)  Among the metals, cadmium is one of the most readily absorbed

                               and accumulated in plants grown in contaminated soil.

                          (4)  The biologic methylation or inorganic lead to tetramethyl lead

                               by lake sediment microorganisms has been demonstrated, but the

                               significance of this observation remains uncertain.

                          (5)  Bioaccumulation of arsenic species occurs readily in some

                               aquatic organisms. Seaweeds, freshwater algae and crustaceans

                               accumulate significant amounts of arsenic. The ambient water

                               concentration (FDA) for arsenic is suggested to be zero to

                               protect human health from potential carcinogenic effects of

                               arsenic exposure through ingestion of water and contaminated

                               aquatic organisms.

                          (6)  Silver is toxic to humans and aquatic organisms at very low

                               concentrations. Once absorbed by living tissues, silver is

                               'not readily removed and tends to accumulate.

                          (7) In general, mollusca, crustaceans, oliqochaetes and leeches

                               appear to be the most sensitive taxa to zinc.

                     B.   State-Wide Summary

                          In order to evaluate and summarize the sediment heavy metal data

                     identified during this study, it is necessary to view the data in two

                     different manners; specific concentrations of heavy metals in sediments

                     and overall location of the sampling sites. The concentrations of metal

                     in sediments is compared with two sets of limitations; USGS and USEPA

                     Region 6 alert levels in sediments, and Statewide Order No. 29-B heavy

                     metals limitations. These are listed in Tables 3 and 4, respectively.

                     The overall location of sample sites is best determined by perusal of

                     the data maps (Appendix A).

                          The following general comments can be made based upon the data

                     listings, the prepared maps and the listings of excursions from the

                     sediment alert levels and 29-B limitations. East of Michoud in Orleans

                     parish there is a cluster of samples taken along the Gulf Intracoastal

                     Waterway, and in feeder tributaries. Of the nine samples taken in this

                     cluster, eight exceed some parameter of the 29-B limitations. Of the

                     twelve sites sampled in Lake Pontchartrain, all exceed 29-B background

                     limits.

                          Random samples were taken along the Mississippi River Gulf Outlet

                     in St. Bernard Parish; from mile 0 to approximately mile 50. At mile 20

                     there is a cluster which extends from the north and south sides of the

                     channel bank out into Chandeleur and Breton Sounds. A majority of these

                     samples exceed 29-B limits. Sites in Plaquemine Parish are also in

                     waterways; a cluster is noted at the mouth of Southwest Pass. All

                     wetland samples at one site of a proposed freshwater diversion structure

                     exceed limitations in 29-B.

                                                                                                   12

                             Table 3. Toxic Criteria and    Alert  Levels for Metals in
                                       Freshwater and Sediments

                                            USGS Alert Levels        Region 6 Alert Levels
                             Parameter        in Sediments            for Sediment (ug/1)
                                                  (ug/kg)           Interstitial/Elutriate)

                             Antimony             500,000
                             Arsenic              200,000                   440 (As +3

                             Barium             2,000,000

                             Beryllium            200,000

                             Boron                   -

                             Cadmium               20,000                  24 hr. Avg.

                             Chromium             200,000  (t)           Max. level 0.29

                             Copper             2,000,000                       5.6

                             Cyanide              100,000                       3.5

                             Iron                    -                           -

                             Lead                 500,000                  24 hr. Avg.

                             Manganese               -                           -

                             Mercury               20,000                        .2

                             Nickel             2,000,000                  24 hr. Avg.

                             Selenium              20,000                        35

                             Silver             1,000,000                  Max.  level

                             Thallium                -                           -

                             Zinc               5,000,000                        47

                             W = total chromium

                              as inorganic selenite

                             1
                              Compiled from DRAFT, Arkansas, Oklahoma, Louisiana, New
                              Mexico, and Texas, Environment Protection Agency, Region 6,
                              Sediment Alert Levels

                                                                                                       13

                             Table 4. State-Wide Order 29-B Limitations for all Pit
                                        Closures and Solidification.

                             Limitations for Waste/Soil
                                Mixtures for all Pit                   Leachate Testing
                                 Closure Techniques                     (EP Toxicity)
                                                                      for Solidification
                             Parameter         Limitation                   (mg/1)
                                                   (ppm)

                             Arsenic                 10            Arsenic          <  0.5

                             Barium               2,000            Barium           <  10.0

                             Cadmium                 10            Cadmium          <  0.1

                             Chromium               500            Chromium         <  0.5

                             Lead                   500            Lead             <  0.5

                             Mercury                 10            Mercury          <  0.02

                             Selenium                10            Selenium         <  0.1

                             Silver                 200            Silver           <  0.5

                             Zinc                   500            Zinc             <  5.0

                                                                                           14

                         Coverage in Jefferson Parish is in waterways only. The majority of

                     samples taken along Barataria Bay waterway exceed some parameter of the

                     29-B limitations. Coverage in St. Charles, St. James, St. John the

                     Baptist, Ascension, Jefferson Davis and Lafayette Parishes can be con-

                     sidered non-existent as none of these parishes has more than 4 samples

                     parishwide; and for the most part, samples were taken in water courses

                     only.

                          All places sampled along the Gulf Intracoastal Waterway in

                     Lafourche and Terrebonne Parishes exceed metal limits for 29-B. The

                     coastal wetland between Jefferson Parish and the Atchafalaya River lack

                     coverage. There are a few samples in small clusters in this area in

                     waterways. One cluster, at the head of the Houma navigation canal and

                     the Gulf Intracoastal Waterway exceeds the 29-B limits. Samples along

                     the Atchafalaya River channel in the Atchafalaya Bay, and samples in

                     Grand Lake, Six Mile Lake, Lake Palourde and Flat Lake also exceed 29-B.

                     Two of the eleven samples in Lake Verret exceed 29-B limits. One

                     sample, Sa.6, exceeds USEPA Region 6 alert levels for cadmium. This is

                     apparently a bad sample as the cadmium levels at th same site for dates

                     previous to, and after the "excess" sample taken, were in an acceptable

                     range.

                          A cluster of eleven samples in the Gulf, Southwest of Chenier au

                     Tigre in Vermillion Parish exceed the limitations of 29-B. Also in the

                     Gulf, the cluster of samples to the south of the old and new Mermentau

                     River channel outlets exceed 29-B. Thirteen of twenty-one samples taken

                     from the Calcasieu Ship Channel, starting at the beginning of the

                     dredged channel to north of Rabbit Island in Calcasieu Lake exceed

                     limits of 29-B. Also above 29-B are samples in the site clusters at

                     Moss Lake

                                                                                           15

                     and site clusters at Lake Charles. Jefferson Davis Parish with three

                     sites and Iberville Parish having six sites were the only two parishes

                     of the twenty-one parishes surveyed that contained sites which did not

                     exceed the 29-B limitations.

                          There is a gross lack of complete parish wide coverage in sampling

                     for metals. Most of the sites were either clustered or at intervals

                     along navigable waterways taken in conjunction with dredging activities.

                     The majority of land area was devoid of any sample sites whatsoever.

                     There is not a consistency of metal specie sampled. Generally, data from

                     storet shows the same metals sampled for each site, but variations in

                     metals do occur. Data from non-federal government agencies or private

                     firms usually sample for only a very limited number of metals. More

                     rapid sedimentation and scour occurs in outlet channels and swift

                     flowing rivers, therefore data in these areas may not be considered

                     valid if not updated on a regular basis.

                                               4. RECOMMENDATIONS

                          As previously stated, the primary objective of the research effort

                     was to compile an inventory of heavy metals data for the Louisiana

                     coastal sediments. It was not the intent of this study to investigate

                     the severity of metal contamination in the Louisiana coastal zone or to

                     review and evaluate Statewide Order No. 29-B with regard to storage,

                     treatment and disposal of nonhazardous oilfield wastes. Based upon the

                     acquisition of the included sediment heavy metal data and the assessment

                     of that data with regard to deficiencies, it was felt that a brief

                     discussion of number of observations and/or recommendations would be

                     appropriate. These discussions fall into four general categories:

                                                                                           16

                          (1) Additional data modification and updating needs directly

                               relating to this report.

                          (2)  Statewide Order No. 29-B pit closure techniques and onsite

                               disposal of nonhazardous oilfield wastes.

                          (3)  Heavy metal contamination in sediments.

                          (4)  Knowledge-based (expert) systems technology for identification

                               of economic and environmentally sound disposal methods.

                          With regard to data modification and updating needs, there are

                     recommendations relating to the developed software package, data file

                     and maps. The maps indicate the location of each sample site

                     identified. The usefulness of these maps to regulatory officials and

                     industry representatives would be significantly increased if overlay

                     sheets with disposal pits locations were added. This would enable

                     interested parties, either closure plan reviewers or pit owners, to see

                     where the available sediment data is in relation to existing or planned

                     waste pits. It would also make areas which are deficient in available

                     or appropriate sediment data, in relation to disposal pit locations,

                     readily identifiable.

                          In order to make the data system more useful and applicable, a

                     regularly scheduled updating of the data base should be performed. This

                     would add data from on-going or future studies and may include new

                     sampling sites or additional results from existing sample locations. In

                     addition, the method of identifying the location of the oilfield waste

                     pits and the sediment sampling location needs to be standardized. The

                     vast majority of available data is located by coordinates, whereas waste

                     pits are often located by identification of township, section and range.

                                                                                           17

                          Most importantly, the usefulness of the developed data base is

                     directly related to how successful DNR is in identifying and informing

                     potential users of its existence and capabilities.

                          With regard to Statewide Order No. 29-B, only a brief discussion

                     of recommendations will be included in this report as this is beyond the

                     scope of this study. In general, it can be stated that 29-B has

                     established an excellent framework for the regulation of treatment and

                     disposal of nonhazardous oilfield wastes. However, there are some needs

                     that should be addressed in order to enhance it implementation. The

                     following comments deals solely with Sec. XV, paragraph 2.7, "Pit

                     Closure Techniques and Onsite Disposal of NOW".

                          Since the selection of a treatment and disposal technique for an

                     oilfield waste pit greatly depends upon the heavy metal content of the

                     pit and metal content of the background sediments, specific requirements

                     with regard to sampling techniques and locations should be addressed.

                     As can be seen from the sediment data presented in this report, addi-

                     tional data collection may be a necessity in many cases. Decisions will

                     need to be made regarding acceptable distance from a waste pit to

                     available background data. Also specific guidelines need to be listed

                     regarding how and where pit and background sediment samples are

                     obtained. Are samples collected at the surface or are samples compo-

                     sites with depth? What is a sufficient distance from the waste pit for

                     a background sample to be taken? At what distance does the sample no

                     longer relate to the background conditions of the pit? These questions

                     need to be addressed.

                          These questions also relate to the need for the regulations to

                     define who is responsible for data collection if there are data

                                                                                           18

                     deficiencies. As previously discussed, major deficiencies do exist

                     in the data and guidance will be necessary to determine what additional

                     data needs to be collected.

                          Finally, the actual feasibility of utilizing the proposed closure

                     techniques needs to be evaluated. It would appear that in the Louisiana

                     coastal zone, burial or trenching and solidification are not feasible

                     alternatives because of the ground water table requirements. Also, end

                     product requirements for different on-site treatment alternatives need

                     to be standardized. Examples are that solidified wastes must meet

                     compressive strength and permeability limitations, but other treatments

                     do not. Additionally, solidified wastes must meet leachate testing

                     limits when other closure methods do not. It is felt that by defining

                     the specific objectives of 29-B that treatment performance criteria can

                     be easily defined.

                          It is widely known that bottom sediments, either in fresh or salt

                     water, act as accumulators of pollutants, particularly heavy metals.

                     Pollutant concentrations several hundreds or thousands of times the

                     overlying water concentration can result. Problems with polluted

                     sediments arise because, first, these sediments (particularly in the

                     coastal zone) are the habitats for many commercial fisheries species,

                     either for part or all of their life cycle. Second, as bottom sediments

                     are eroded and moved, either naturally or through man induced processes

                     such as dredging, the sediments may act as a source of concentrated

                     pollutants for aquatic organisms and ultimately humans. Finally, the

                     ability to determine the significance and degree of heavy metal contami-

                     nation in bottom sediments is essentially limited to the comparison of

                     absolute metal concentration values alone, which does not account for

                                                                                           19

                     the many physical and chemical sediment parameters that influence

                     sediment metal concentration values.

                         The Louisiana coastal zone is an area containing thousands of

                     square miles of estuaries, which are among the most productive private

                     and commercial fish and wildlife habitat areas in the nation. Excessive

                     heavy metal contamination of these ecologically sensitive estuaries

                     could evoke serious consequences. Initially, the more primitive

                     organisms at the bottom of the food chain would succumb to the

                     contamination. However, once this food chain foundation is eroded, the

                     higher forms of life, including man, could be threatened. However, a

                     sediment contamination threshold, distinguishing an uncontaminated

                     sediment from a contaminated one, has not been established.

                          Several things are needed to mitigate the adverse effects of sedi-

                     ment borne pollutants. First, a knowledge of the present distribution

                     of polluted sediments, including the areal and vertical distribution of

                     pollutant type and amount, is needed. Second, the degree of sediment

                     contamination must be established. Third, knowledge of the processes

                     controlling pollutant concentrations and of the physical/chemical

                     behavior of the adsorbed pollutants is necessary. Fourth, technology is

                     required that will allow bottom sediment pollutants to be accurately and

                     quickly surveyed, to make predictions of future pollutant concentrations

                     and distribution, and to allow pollutant concentrations to be modified

                     or controlled. With the abilities described above, a management of

                     bottom sediment pollutants could be feasible. The problem at present is

                     that the above abilities are not adequately in existence.

                         Current technologies and analytical techniques make the analysis of

                     heavy metals in sediment a routine practice. However, the determination

                                                                                           20

                     of whether significant contamination exists is an unresolved problem.

                     Metal distribution in sediments is influenced greatly by several sedi-

                     ment characteristics, principally grain size and organic content.

                     Because of these influences, dissimilar sediment types have vastly

                     different thresholds of contamination. Currently, the acceptable method

                     of determining heavy metal contamination in sediments involves the com-

                     parison of metal concentration values. However, in some cases, this

                     method can be significantly influenced by a sediment's physical and

                     chemical composition.

                          Presently, efforts to eliminate the influences of heavy metal

                     distribution in sediment are met with varying degrees of moderate

                     success. Procedures to reduce the effects of grain size and organic

                     content on heavy metal distribution in sediment are not only time

                     consuming, but differ widely from researcher to researcher.

                          In natural sediment systems, elements as well as metals exist

                     together in fixed proportions to each other, with only minor variation.

                     Furthermore, some metals are conservative in nature; that is, they are

                     naturally present in soil and sediment in high concentrations and are

                     affected minimally by man-made influences. Trace metals, on the other

                     hand, are naturally present in small concentrations and are greatly

                     affected by man-made influences. Ratios of trace metals to conservative

                     elements reveal geochemical imbalances due to elevated trace metal

                     concentrations normally associated with man-made activities.

                          Correlations do exist between the concentrations of several metals,

                     especially Cd/Fe, Ni/Fe, Zn/Fe and Pb/Al. The significance of these

                     correlations is that it shows there is a similarity between the

                     geochemical cycles in which metals participate. It also implies that

                                                                                           21

                     elements should naturally exist in sediments in relatively constant

                     proportions to one another.

                          Relative atomic variation, a statistical method of determining

                     metal contamination based on regression analysis of significant element

                     pair correlations, does not achieve the success necessary to be

                     considered a viable alternative to the present methods used in

                     determining metal contamination.

                          A better method of analyzing sediments in order to determine con-

                     tamination may be in the use of metal pair concentration ratios alone or

                     in conjunction with the more conventionally accepted method of comparing

                     metal concentration values. Metal pair ratios can be used to determine

                     background metal concentrations and to determine, via comparison, the

                     existence of metal contamination in bottom sediment samples.

                          It is apparent that many non-hazardous oil field waste generators

                     are becoming more confused about their legal and regulatory obligations

                     and about how to select the technically best and most cost effective

                     methods available for properly handling their waste problems. The use

                     of knowledge-based (expert) system should assist generators in their

                     decision making process, be of economic benefit to industry, and help

                     identify environmentally sound waste management options.

                          Prescriptive/consultative knowledge-based systems are an appro-

                     priate means for transferring state-of-the-art treatment and disposal

                     technology and management options to reach world applications.

                          Currently, the public, regulatory agencies and waste generators

                     have difficulties in keeping abreast with the ever changing rules,

                     regulations and technological advances of waste management. An expert

                     system can be a useful means to help solve the problem of keeping

                                                                                            22

                     current with a fast changing technology and to assist regulators and

                     generators in selecting the most environmentally safe and cost-effective

                     waste management approach.

                          The development of expert systems is an advance in computer

                     technology that has taken a special place in the toolkit of systems

                     developers. The use of programming languages such as LISP or PROLOG or

                     a development tool such as ROSIE offer many advantages over conventional

                     programming. The data structures and program control structures have

                     the same syntax and they can be easily updated without major system

                     revisions. This is important in the area of waste management, for any

                     expert system must be one that can be readily updated and be used by a

                     wide range of both technical and regulatory personnel.

                          The prototype system could be developed and tested using both

                     hypothetical and real situations. It would be provided to Louisiana

                     Department of Natural Resources and Office of Conservation staff for use

                     and comment.

                          An expert system could be used to take into account a number of

                     factors, both environmental and economic, which are presently beyond the

                     scope of 29-B. These factors may include items such as distance to

                     nearest permitted commercial disposal facility, risk associated with

                     transportation, background contamination levels, etc. The use of an

                     expert system, together with the background heavy metal data and an

                     approach used to evaluate what the background sediment data means, will

                     make implementation of Statewide Order No. 29-B an important part of

                     protecting Louisiana's natural resources.

                                                                                            23

                              5. REFERENCES, COMMENT LEGEND AND LIST OF SYMBOLS

                    1.   United State Geological Survey, Storet. United States Environ-

                         mental Protection Agency, Washington, D.C., Oct., 1986.

                    2.   United States Army Engineers, New Orleans, District, Storet.

                         United States Environmental Protection Agency, Washington, D.C.,

                         Oct., 1986.

                    3.   U.S. Environmental Protection Agency, Region 6, Storet. United

                         States Environmental Protection Agency, Washington, D.C., Oct.,

                         1986.

                    4.   U.S. Environmental Protection Agency Headquarters, Storet.

                         Washington, D.C., Oct., 1986 (Louisiana Data).

                    5.   Texas Dept. of Water Resources, Storet. United States Environmental

                         Protection Agency, Washington, D.C., Oct., 1986.

                    6.   Atchafalaya Bay Louisiana Sediment and Water Quality Assessment.

                         Corps of Engineers, New Orleans District, New Orleans, LA, July,

                         1975

                    7.   Houma Navigation Canal, Louisiana, Assessment of Impacts of

                         Maintenance Dredging on Water Quality. Corps of Engineers, New

                         Orleans District, New Orleans, LA, July, 1975

                    8.   Barataria Bay Waterway, Louisiana, Assessment of Impacts of

                         Maintenance Dredging on Water Quality. Corps of Engineers, New

                         Orleans District, New Orleans, LA, July, 1975

                    9.   Atchafalaya Basin East and West Access Channels and West Freshwater

                         Distribution Channel, Assessment of Impacts of Maintenance Dredging

                         on Water Quality. Corps of Engineers, New Orleans District, New

                         Orleans, LA, July, 1975

                                                                                          24

                    10. Devel, Lloyd E., Jr., and Zahray, R. K., "Final Report -

                          Demonstration of Drilling Mud Waste-Wetland Soil Compatibility."

                          July 1983, Shell Oil Co.

                    11.   Data from Subra Co. Waste Pits in Vermillion Parish. New Iberia,

                          LA.

                    12.   Twelve Month Interpretive Data Report on the St. Rosalie Site.

                          Gulf South Research InstituteV LA, Jan. 1977.

                    13.   Collection and Analysis of Sediment Samples Maintenance Dredging

                          Material, Navigation Projects. Mobile District, Corps of

                          Engineers, Jan. 1977.

                    14.   White, Kevin D. and Tittlebaum, Marty E., "Metal Distribution and

                          Contamination in Sediments." ASCE, Journal of Environmental

                          Engineering, April 1985.

                    15.   Analysis of Water, Core Material, and Elutuate Samples Collected

                          Near Buras, Louisiana. Harold L. Leone, Jr., U.S. Dept. of the

                          Interior, Geological Survey, April 1977.

                    16.   Analysis of Water, Core Material, and Elutuate Samples Collected

                          Near New Orleans, Louisiana. U.S. Dept. of the Interior,

                          Geological Survey, 1977.

                    17.   Environmental Assessment for Unauthorized Forced Drainage Project.

                          Environmental Industrial Research Associates, Inc., Metairie, LA,

                          May 1984.

                    18.   Winger, P. V. and Andreaseu, J. K., "Contaminant Residue in Fish

                          and Sediments from Lakes in the Atchafalaya River Basin

                          (Louisiana)." Archives of Environmental Contamination and

                          Toxicology, 1985.

                                                                                           25

                     19. DeLaune, R. D., Reddy, C. N. and Patrick, W. H., Jr., "Accumulation

                          of Plant Nutrients and Heavy Metals through Sedimentation Processes

                          and Accretion in a Louisiana Salt Marsh." Estuaries, December

                          1981.

                     20.  Research Triangle Institute - Final Report - Analysis of Metals and

                          Organics in Sediment and Biota. March 18, 1985.

                     21.  U.S. Army Engineers, Vicksburg District, Storet. U.S.

                          Environmental Protection Agency, Washington, D.C., Oct. 1986.

                     22.  U.S. Environmental Protection Agency Headquarters, Storet. Texas

                          Data, Washington, D.C., Oct. 1986.

                     23.  Ecology and Environment, Inc., Dallas, Texas. Pit Sampling at D.

                          L. Mud, Inc., Abbeville, LA, June, 1986.

                     24.  Ecology and Environment, Inc., Dallas, Texas. Pit Sampling at D.

                          L. Mud, Inc., Abbeville, LA, July, 1985.

                     25.  Holder, S. W., Jr., "Selected Trace Elements in the Water,

                          Sediment, Particulates and Estuarine Clam, Rangia Cuneata, from

                          Lake Pontchartrain, Louisiana." M.S. Thesis, UNO, New Orleans,

                          1979.

                     26.  Environmental Impact Statement - Southwest Pass, Mississippi River

                          Ocean Dredged Material Disposal Site Designation. EPA - Office of

                          Water Criteria and Standard Division, Washington, D.C., Aug. 1984.

                     27.  Heavy Metal Inputs to Mississippi Delta Sediments - A Historical

                          View. B. J. Presley, J. H. Trefry and R. F. Shokes, 1980.

                     28.  Khalid, R. A., Gambrell, R. P., Taylor, B. A. and Patrick, W. H.,

                          "Literature Survey of Reservoir Contaminant Problems," Laboratory

                          for Wetland Soils and Sediment, Center for Wetland Resources, LSU,

                          Contract No. DACW 39-80-C-0032, May 1983.

                                                                                               26

                                                   COMMENT LEGEND

                     g.    ppm (parts per million)

                     h.    elutriate data may be available

                     i.    other metal data may be available

                     j.    water column data may be available

                     k.    actual value is known to be less than value given

                     1.    actual value is known to be greater than value given

                     M.    presence of material verified but not quantified. In the case of

                           temperature or oxygen reduction potential, M indicates a negative

                           value.

                     n.    mg/g (milligram per gram)

                                                   LIST OF SYMBOLS

                     Ag    silver                         Fe   iron

                     Al    aluminum                       Hg   mercury

                     As    arsenic                        Mn   magnesium

                     Ba    barium                         Ni   nickel

                     Be    beryllium                      Pb   lead

                     Cd    cadmium                        Se   selenium

                     Co    cobalt                         V    vanadium

                     Cr    chromium                       Zn   zinc

                     CU    copper

                                                                                            27

                                                6. BIBLIOGRAPHY

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                     Andren, A. W. and Harriss, R. C., "Methylmercury in Estuarine
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                     Connell, D. W. and Miller, G. J., Chemistry and Ecotoxicology of
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                     Gouguet, R., Department of Wildlife and Fisheries, Seafood Office, Baton
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                                                                                                29

                      Grantham, C. K. and Sloan, J. P., "Toxicity Study Drilling Fluid
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                      Isphording, W. C., Flowers, G. C. and Stringfellow, S. A., "Comparison
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                      Klaassen, C. D., Amour, M. 0. and Dovll, J., Toxicology, MacMillian
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                                                                                           30

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                                                                                             31

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                                                                                            32

                     Warren, J., U.S. Army Engineers, Hydraulics Section Engineering
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                                                   APPENDIX C

                                 Excursions from USGS Sediment Alert Levels and
                                        Statewide Order 29-B Limitations

                                    Sites and Metals Exceeding USEPA Region 6
                                               Sediment Alert Levels:

                                               sa. 6
                                          Cd     80010.00

                                                     S
                                                     L
                                                        ites and Metals Exceeding Statpwide Order '.7-19-B
                                                                                   Sec. '2."'.C.2 Limitations

                                                                        s a n . 2*@                                                           so.5
                                                                 C d          I C) . 0 0

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                                                                 Cd           1 0 .     0                                             As                5 1-.-
                                                                 Pb           5 C) C)   C.) 0
                                                                 A s          20.0C)
                                                                                                                                              sp. 4
                                                                                                                                      As           I C). C.)0
                                                                        sa. 6
                                                                 As           I I . 00
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                                                                        sca. 5                                                        As           12. 0
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                                                                        sca. 6                                                                cp. 2
                                                                 As           12). C)C)                                               As           12. 00
                                                                                                                                      C* d         I C). 0 0 k.

                                                                        sca. 7
                                                                 As           10. 00                                                          cp. 3
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                                                                        sca. 8
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                                                                 Cd           10 . 0 C.) k:
                                                                 As           11. Oo
                                                                 Cd           I o. 0 C) tf.                                                   sb.7
                                                                                                                                      As           I C.). C)C)

                                                                        sc.5
                                                                 As           16. Oo                                                          sb.13
                                                                 Cd           I C). () 0 k                                            As           I (). 00
                                                                 As           1    0 0                                                Cd           I C). C) 0 k
                                                                 Cd           1

                                                                                                                                              sb.14
                                                                        sc.6                                                          As           11. 00
                                                                 As           15.00
                                                                 Cd           I C) . (:) C)
                                                                 As           I C). 00                                                        sb.15
                                                                 Cd           1. C). 0 C-) k                                          As           I C). OC-)
                                                                                                                                      Cd           10. C) 0 k

                                                                        sc.7
                                                                 As           16.00                                                           sb.16
                                                                                                                                      As           10. 00
                                                                                                                                      Cd           10. 0 0 k...
                                                                        sc.8
                                                                 As           14. 00
                                                                                                                                              sch.1
                                                                                                                                      As           I().
                                                                        sc.9                                                          Cd           I C-). Cj C)
                                                                 As           19.00                                                   As           12). 00
                                                                 Cd           I C). C) C) kl

                                                                                                                                              hch.1
                                                                        sc. IC-)                                                      As           37. 91-::
                                                                 As           2@3. Oo

                                                                                                                                              si m. 3
                                                                        sc.11                                                         Cd           I C). 0 0 k:
                                                                 As           2 2 . 0 C)

                                                                                                                                              smn.
                                                                        sc. 12                                                        Cd           1. 0   C.) 0
                                                                 Os           10.00

                                                                                                                                             smn. 4

                                                                Pis          1 r@, . C) C)                                            C-; d        10 . C) C)

                                                                        sc-.14                                                               sain. 9
                                                                As           19. c)(..)                                               Cd           I C). 0 C) I.-..

                                                                        !:-,c. 1.5                                                           sain. 10
                                                                As           .14. 00                                                  Cd           10 . 0 C
                                                                Cd           I C.). o C)
                                                                As           13. Oo
                                                                Cd           10. oo                                                          smn. 1'3
                                                                                                                                      Cd           I C) . (7) C.) k

                                                                        sc. 16
                                                                cd           I C). 0 0 1...                                                  smn. 15
                                                                Cd           10. 0 C)                                                 Cd           I o. 00

                                                                        sc:.17                                                               smn.16
                                                                As           I                                                        Cd           10. 00 k

                                                                        sc.18                                                                smn.1",
                                                                Cd           I C) . C) 0 1-::                                         Cd           10. 0 C)
                                                                As           12. 0 C)
                                                                cd           10 . 0 ('-') k
                                                                                                                                             smn.18
                                                                                                                                      As           I C). (-)C)
                                                                        sc.19                                                         Cd           I C-). 0 0
                                                                As           17. C) 0

                                                                                                                                             smn.'2o
                                                                        sc. 2C)                                                       Cd           1         C.) C)
                                                                As           131. 00

                                                                                                                                             sm. 6
                                                                        sc.21                                                         Cd           I C). C) 0
                                                                As           18.00

                                                                                                                                             sm.'7
                                                                        sc.22                                                         Cd           1 (). OC-) k
                                                                As           14. Q C-)

                                                                                                                                             sm. 10
                                                                        sc.23                                                         As           14. C)o
                                                                As           14.00

                                                                                                                                             sm. 1,X2,
                                                                        sc.24                                                         Cd           I C-) . 0
                                                                As           15.00

                                                                                                                                             sm.13
                                                                        i=-,c . '2@6                                                  Cd           I o. () C-) I-..-
                                                                As           16. (--)C)

                                                                                                                                             sm. 14
                                                                       sc.                                                            Cd          1 C). C) C) k
                                                                As           I I. C)
                                                                Cd           I C) @ C) C) k

                                                                                                                                      Cd          I C). C) C-)
                                                                               -@9
                                                                cd           .1 C). f.:)
                                                                Cd           10. C)C)i-.-.                                                               I
                                                                                                                                      Se          22. 'X2

                                                                       sc.
                                                                Cd           I     OCC                                                       rtm. 2
                                                                                                                                      As          I(). C-) k.
                                                                                                                                      Se          20.
                                                                       T,c . 38
                                                                As           13 . 0 C)
                                                                                                                                             rtm. 3
                                                                                                                                      As          13. 1
                                                                       sc. 39                                                         As          70. 1
                                                                As           10. oc)                                                  Se          2 0. 0

                                                                       sc. 4C)                                                               sty. I
                                                                As           12. C.)C-)                                               Cd          10. f") C) k.

                                                                       sc.42                                                                 sty.2,
                                                                Ccj          10. OOL                                                  Cd          10. 0 0 k:

                                                                       sc.43                                                                 sty.3
                                                                cd           I C-). OOL                                               Cd          I C-) .  0 1-.-.

                                                                       sc.50                                                                 sty.4
                                                                Cd           10. 0 0 k:                                               Cd          10. Oo k
                                                                Cd           I C-). C-) 0 k

                                                                                                                                             cty.1
                                                                       sc.51                                                          Cd          I C) @ C) 0 k
                                                                As           12. 0 C)
                                                                Cd           10. 00k.
                                                                As           12.00                                                           hty.1
                                                                                                                                      As          3, 8 . C)

                                                                       rtc.1
                                                                As           10. 0                                                           hty.2
                                                                Se           4B.9                                                     As          38.61-::
                                                                As           10 . 0 k:
                                                                Se           ")C .
                                                                                                                                             hty. 3
                                                                                                                                      As          "R. 6k:

                                                                       As;           I
                                                                       cd            I C)      C)                                                           St. I
                                                                                                                                                     Cd           I C)   C) 0 k

                                                                               is i
                                                                       Cd            I
                                                                                                                                                               t
                                                                                                                                                            S
                                                                                                                                                     As           t CID
                                                                                                                                                     Pb                C C)   C) C)
                                                                                                                                                     Zn           54C).
                                                                       A s           10. 00                                                          A ss         17.
                                                                       C' d          I                                                               Pb           140C).
                                                                       As            15. 00                                                          Z n          560. 00
                                                                       Cd            10 . C)

                                                                                                                                                            St. :3
                                                                               si . 4                                                                As           11 . C)O
                                                                       Cd            1      0 0                                                      Cd           I Q . 0 0
                                                                       As            10. 00                                                          As           17. C) 0
                                                                                                                                                     Cd           I C) . C) C)

                                                                               si . 5
                                                                       As            12. 0C.)                                                               St. 4
                                                                       Cd            I (--) . C) C)                                                  As           .2 1 . C-) 0
                                                                       As            IC). 00                                                         As           3-r 2 . 0 C.)
                                                                       Cd                   C.) C-)

                                                                                                                                                            St. 5
                                                                               Si . 6                                                                A            I C-). C)C)
                                                                       As            15. 00
                                                                       Cll d                   C)
                                                                       Ass           17. 00                                                                 St. 6
                                                                       cd            10 . C) C)                                                      As           I C). (:)C)

                                                                               si . 7                                                                       St. -7
                                                                       Cd            I C.). C-) C)                                                   As           16.00

                                                                               Si . 10                                                                      St. IC)
                                                                       Cd            I C) . C-) C) k                                                 As           13. 0 C)

                                                                               Si . 8                                                                       St. I I
                                                                       Cd            10 . 0 C)                                                       As           I I . 00
                                                                       Pb            5 C) 0 0 .
                                                                       AS            10. OC)
                                                                       As            10. 00                                                                 St. 12
                                                                                                                                                     A S          1 C) . 0 C)
                                                                                                                                                     As           11.0o
                                                                               Si . I
                                                                       As            I I . OC)
                                                                       As            10 . C)                                                                c t . 77
                                                                                                                                                     AS           1"::.. 0C.)L

                                                                        si . 2
                                                                As            1 '2  C)                                                       ct. 4
                                                                As            1     C)
                                                                                                                                      As          122. OOL.
                                                                Pis           I     C)C)

                                                                                                                                             eirt. I
                                                                        s 71
                                                                          j ",.-:                                                     Cd          2 C       0 C) 1.::
                                                                As            10. Oo                                                  Ficl        6 8 (8 .
                                                                As            I';. C-) C)                                             Flb         .15 4 C)      C) C) k.
                                                                As            I     C) 0                                              AZ n        '71800.

                                                                        s.j . 7                                                              eirt.2
                                                                As            10. C)O                                                 Cd          41C)
                                                                                                                                      Hq          1-78
                                                                                                                                      Pb          5 0 0 k
                                                                        sj .9                                                         Zn          65700
                                                                As            14. 00

                                                                                                                                             ei rt.'.%'
                                                                        cj . I                                                        Cd          42C)
                                                                                                                                                  .8C
                                                                As            11.00                                                   Hg          I -)
                                                                As            I     C) C-)                                            Pb          127(--)(-)
                                                                                                                                      Z n         144 100

                                                                        c.i
                                                                As            12. 00                                                         ei rt. 4
                                                                As            I                                                       Cd          42C)
                                                                                                                                      Hg          le(')
                                                                                                                                      Pb          l'270C)
                                                                                                                                      Z n         144 1 C)C)
                                                                As            3 9. C-)

                                                                                                                                             rtt. I
                                                                        h.j . 2                                                       Be          49.8
                                                                As            39.1k.                                                  As          49.5
                                                                                                                                      Be          20. 0 1..-.

                                                                        hi . 31
                                                                As            4 0. 3 k:                                                      r t t . 2@
                                                                                                                                      Cd          603

                                                                        hi.4
                                                                As            4C). 1 k:                                                      rtt.4
                                                                                                                                      As          10.7
                                                                                                                                      Be          6 7 .  0
                                                                        hi.5                                                          As          12.3.
                                                                As            122k.                                                   As          IC). (.-) @-.-
                                                                                                                                      Be          2 C). C) 1,.*

                                                                        hi.6
                                                                As            112k.                                                          rtt.5
                                                                                                                                      Be          3B. 4
                                                                                                                                      As          49.8
                                                                        h                                                                         "%', C).
                                                                          j . 7                                                       Se,
                                                                As            116 k:

                                                                                                                                              stx . I
                                                                        S.1 a.                                                         As          I     C) C)
                                                                 Cd           10.       k.                                             As          -36.
                                                                 C" d         1     C) C)                                              As          16. 00
                                                                 A s          23. C)O                                                  As          @2,5. 0C)

                                                                        S1.1                                                                  s t      -3
                                                                 As           I I . 0(.-)                                              Cd          10. k'*-')()L
                                                                 Cd           I U.    VI.,

                                                                                                                                              st,x . 7
                                                                        sl . 4                                                         As
                                                                 As           16. Oo
                                                                 As           14.
                                                                                                                                              stx      IC)
                                                                                                                                       As          15. 00
                                                                        sl.5
                                                                 As           10. OC)
                                                                                                                                              stx. 12
                                                                                                                                       As          20. OC)
                                                                        sl.6
                                                                 As           10. OC-)
                                                                                                                                              sv. I
                                                                                                                                       As          14. C-)0
                                                                        sl.7                                                           Cd          I C). C) () @.'.
                                                                 Cd           I C.). 0 () k.                                           As          11. 00
                                                                                                                                       Cd          I C). 0 0 k

                                                                        sl . 10
                                                                 As           14.00                                                           s v . 2.
                                                                                                                                       As          14. 0 C-)
                                                                                                                                       Cd          1 o. 00k.
                                                                        S1.11
                                                                 As           1 12) . 0 C)
                                                                 As           11. 00                                                          sv.3
                                                                                                                                       As          2 1. 00
                                                                                                                                       Cd          10. 00k
                                                                        rt I . I
                                                                 Cd           404.0
                                                                 Se           50.6                                                            sv. 4
                                                                 Cd           707@*. C)                                                As          2 5. C) 0
                                                                 As           I (). Ok                                                 Cd          I C). Oot....
                                                                 Se           20. C)k

                                                                                                                                              sv. 5
                                                                        sc-j. 4                                                        As          13 @ 00
                                                                 As           1 C). 00                                                 Cd          10. 00 k.
                                                                                                                                       A i---,     12. C-)0
                                                                                                                                       Cd          10. 0 0
                                                                        so. 7
                                                                 As           12. 0
                                                                 As           I C). 00                                                        sv. 6
                                                                                                                                       A s         10. Oo
                                                                                                                                       As          14. 00

                                                                PIS          11    0 C)
                                                                C d          10    C) C) k                                                   s -v
                                                                                                                                      A s
                                                                                                                                      C d          I C). 0 0 k.

                                                                A s          IC).
                                                                C d          I C).   0 k,                                                    sv. 8
                                                                                                                                      As           1.5. C-)C)
                                                                                                                                      Cd           I        C)
                                                                        so. I IT
                                                                Cd           10. 0 C)
                                                                As           I C). c)(...)                                                   sv. 9
                                                                                                                                      As           2 -,]F . C) C-)
                                                                                                                                      C d          10. 00 k
                                                                        so.16
                                                                Cd           I        C)
                                                                                                                                             sv. 10
                                                                                                                                      As           19. 0 C)
                                                                        so.17                                                         Cd           I C). C) () k
                                                                Cd           10. 0 C) k                                               Cd           I C). 0 0 k.

                                                                        so.18                                                                sv. 11
                                                                Cd           10 . 0 C')                                               As           11. 00
                                                                                                                                      Cd           10. OC) k
                                                                                                                                      cd           10. 0 0 k:
                                                                        so.19
                                                                cd           10. () 0 k.
                                                                                                                                             sv. 13
                                                                                                                                      As           171. C 0
                                                                        so. 20                                                        Cd           IC). 00 1.:'
                                                                Cd           10. OC) k                                                As           19. C)O
                                                                                                                                      Cd           1 C). C) 0 k:

                                                                        so.21
                                                                As           15.00                                                           ev. 2
                                                                As           16. 00                                                   Ba           '2 5 0 C-) . C-) C.)
                                                                                                                                      As           2 0 . k'-") 0
                                                                                                                                      Ba           860(). 00
                                                                        so . 27,3                                                     Zn           160C). 00
                                                                Cd           1 C). 00

                                                                                                                                             e v .
                                                                        so.24                                                         As           I C). (-)C)
                                                                Cd           10. 00k.                                                 Ba           2500. 00
                                                                                                                                      Zn           110 () . C) 0
                                                                                                                                      As           71 . 00
                                                                        so.26                                                         Ba           1. 0000.
                                                                Cd           1(--). 00 k                                              Cd           11.00
                                                                                                                                      Pb           I I Oo. Oo
                                                                                                                                      Zn           7800. 00
                                                                        so.12
                                                                As           11. 00
                                                                                                                                             rtv. I
                                                                                                                                      Se           42.6
                                                                                                                                      As           11.8

                                                                   Iiiiimiiiiiliiiiiiil@
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