A LABORATORY STUDY OF SOLIDIFICATION/STABILIZATION

TECHNOLOGY FOR CONTAMINATED DREDGED MATERIAL!

bvJames Michael Betteker

Thesis submitted to the Faculty of the

Virginia Polytechnic Institute and State University

in partial fulfillment of the requirements for the degree of

Master of Science

in

Environmental Science and Engineering

APPROVED:(

jr . errar , Co-C airman D. D. Lu wig, Co C man

‘

srT.Novat/ ‘/ “

March, 1986

Blacksburg, Virginia

A LABORATORY STUDY OF SOLIDIFICATION/STABILIZATION

TECHNOLOGY FOR CONTAMINATED DREDGED MATERIAL

byJames Michael Betteker ‘

Committee Chairmen: Joseph H. Sherrard

and Daniel D. Ludwig

Environmental Science and Engineering

(ABSTRACT) ‘

Safe disposal of contaminated dredged material has be-

come a significant issue especially as public environmental

awareness and concerns increase. Solidification/ stabiliza-

tion technology potentially may provide for a safer, more

effective and more economical means of disposal.

This research investigated the technical feasibility ofl

applying solidification/stabilization technology to contam-

inated sediment from Indiana Harbor Canal, Indiana. Specif-n

ically, physical strength and reduction of chemical

leachability resulting from solidification/stabilizationA

with various cement based, pozzolanic, and proprietary addi-

tives were analyzed. Also investigated was the

immobilization capability of a proprietary polymer for se-

lected organic contaminants when used in conjunction with

solidification/stabilization processes.

Physical strength is an important parameter in deter-

mining the ultimate bearing capacity, stability of

embankments and pressure against retaining walls. Physical

stabilization of contaminated dredged material is a viable

treatment option. Application of cement-based andIpozzolanic—based processes uses the sediment moisture to form

hydration products, therefore dewaterimg is not required.

All process formulations produced a solidified sediment.

The chemical stabilization tests were conducted using a

modification of the proposed EPA Solid Waste Leaching Proce-

dure (SWLP) as modified by the U.S. Army Corps of Engineer

Waterways Experiment Station. No one process formulation

proved to be effective in providing chemical stabilization

for arsenic, metals, total organic carbon, or organics.

Solidification did provide a significant amount of chemical

stabilization. Aqueous phase concentrations were lower than

sediment phase concentrtions by as much as three to five or-

ders of magnitude and in many cases contaminants were com-

pletely immobilized.

ACKNOWLEDGEMENTS

The author would like to acknowledge the following per-

sons for their help in completing this research:

Dr. Joseph H. Sherrard and Dr. Daniel D. Ludwig fortheir support and supervision as co-chairmen ag the author'sgraduate committee.

providing the opportunity to work with him cui this researchproject. _ -

Dr. John T. Novak for serving on the author's committee

and most importantly for his assitance in getting the authorinto the Environmental Science and Engineering program at

VPI&SU.S

Dr. John Harrison, Dr. Ray Montgomery, and the U.S. ArmyCorps of Engineers Waterways Experiment Station (USAE WES),

Vicksburg, Mississippi, for providing the author the oppor-tunity of working on this research project and the use oftheir facilities. This work was sponsored by on-going re-search at USAE WES for the U.S. Army Engineer District,

Chicago, Chicago, IL.

. iv

V .

TABLE OF CONTENTS

EEABSTRACT ...................... ii

E

ACKNOWLEDGEMENTS . . . ............... ivLIST OF TABLES ................... viAPPENDIX LIST OF TABLES .............. ix

LIST OF FIGURES .................. xiii

CHAPTER

l. INTRODUCTION ................ l

Objectives ............... 6

Approach ....... - ·-·•----. 62. LITERATURE REVIEW ............. 7

Solidification/Stabilization Tech-nologies for Hazardous Waste ...... 7Solidification/Stabilization Tech-nologies for Dredged Material ...... 16Test Procedures for Physical-ChemicalEvaluation of Solidified/Stabilized4 Products .............._. . 20

3. MATERIALS AND METHODS ........... 34

Materials ................ 34

Experimental Design ........... 37

Laboratory Procedure .......... 40

g Sample Processing .......... 40

Unconfined Compressive StrengthTesting ............... 40

_ vi

IPage

2 Serial Batch Leach Testingfor Metals and Total Organic Carbon . 4l

Serial Batch Leach Testingfor Polyaromatic Hydrocarbons andPolychlorinated Biphenyl Congeners . . 43

Analytical Laboratory Group Analysisof Leachate and Sediment ....... 44Determination of Contaminant Concen-tration in Leachate and Sediment . . . 46

4. RESULTS AND DISCUSSION ........... 50Results ................. 50

Physical Stabilization ........ 50Chemical Stabilization ........ 57

Discussion ............... 59Physical Stabilization ........ 59Chemical Stabilization ........ 61

Arsenic and Metals ........ 62Total Organic Carbon ....... 69Polyaromatic Hydrocarbons andPolychlorinated Biphenyls ..... 72

Relationship Between Physical andChemical Stabilization ........ 81

5. CONCLUSIONS ................ 82LITERATURE CITED .................. 84APPENDIX ...................... 91VITA ........................ 116

vii

LIST OF TABLES

Table Page

I. Advantages and Disadvantages of Cement- 'Based Processes ................ 11

II. Advantages and Disadvantages of Lime—Basedand Pozzolanic Processes ........... 12

III. Standard Test of Physical Properties ..... 23IV. Unconfined Compressive Strength of Various

Materials ................... 26

V. Comparative Analysis of Indiana Harbor andLake Michigan Sediments ............ 35 4

VI. Solidification/Stabilization Process MixRatios .................... 38

VII. Process Mix Ratios for Chemical Leaching ofPolyaromatic Hydrocarbons and PolychlorinatedBiphenyl Congeners .............. 39

VIII. Contaminant Concentration in the Sediment 7Before Solidification ......._...... 49

IX. Analysis of Arsenic and Metals Leachate DataShowing Significant Contaminant Immobiliza— .tion ..................... 63

X- Process Effectiveness of Solidification/Stabilization Formulations for Total OrganicCarbon .................... 73

XI. Classification of Data for PolyaromaticHydrocarbons from Serial, Graded Batch LeachTests Conducted on Solidified ContaminatedDredged Material ............... 75

XII. Classification of Data for PolychlorinatedBiphenyl 1248 Congeners from Serial, GradedBatch Leach Tests Conducted on SolidifiedContaminated Dredged Material ......... 76

viii ·

APPENDIX LIST OF TABLES

Table Page

A-I. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with l0 PercentPortland Cement .............. 92

A-II. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 20 PercentPortland Cement .............. 93

A-III. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 30 PercentPortland Cement .............. 94

A—IV. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 40 PercentPortland Cement .............. 95

A-V. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 40 PercentFIRMEX ................... 96

A-VI. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 50 PercentFIRMEX ................... 97

A—VII. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 60 PercentFIRMEX ................... 98

ix

Table Page

A—VllI. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 20 PercentFIRMEX and 10 Percent Portland Cement . . . 99

· A—lX. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 10 PercentFIRMEX and 20 Percent Portland Cement . . . 100

A-X. Contaminant Immobilization Data on yArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 15 PercentFIRMEX and 15 Percent Portland Cement . . . 101 .

A-XI. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 1 PercentPolymer and 20 Percent Portland Cement . . . 102

A-XII. Contaminant Immobilization Data on— Arsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 3 PercentPolymer and 20 Percent Portland Cement . . . 103

A—XllI. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 5 PercentPolymer and 20 Percent Portland Cement . . . 104

A—X1V. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 1 PercentPolymer and 50 Percent FIRMEX ....... 105

A-XV. Contaminant Immobilization Data ong Arsenic, Metals, and Total Organic Carbon

for Contaminated Dredged MaterialSolidified/Stabilized with 3 PercentPolymer and 50 Percent FIRMEX ....... 106

· x

Table Page

A—XV1. Contaminant Immobilization Data onArsenic, Metals, and Total Organic Carbonfor Contaminated Dredged MaterialSolidified/Stabilized with 5 PercentPolymer and 50 Percent FIRMEX ....... 107

A—XVI1. Contaminant Immobilization Data onPolyaromatic Hydrocarbons for ContaminatedDredged Material Solidified/Stabilizedwith 20 Percent Portland Cement ...... 108

A-XVIII. Contaminant Immobilization Data onPolyaromatic Hydrocarbons for ContaminatedDredged Material Solidified/Stabilizedwith 3 Percent Polymer and 20 PercentPortland Cement .............. 109

A—X1X. Contaminant Immobilization Data onPolyaromatic Hydrocarbons for Contaminated _Dredged Material Solidified/Stabilizedwith 50 Percent FIRMEX ........... 110

A—XX. Contaminant Immobilization Data onPolyaromatic Hydrocarbons for ContaminatedDredged Material Solidified/Stabilizedwith 3 Percent Polymer and 50 PercentFIRMEX ................... 111

A—XXI. Contaminant Immobilization Data onPolychlorinated Biphenyl 1248 Congenersfor Contaminated Dredged MaterialSolidified/Stabilized with 20 PercentPortland Cement .............. 112

A-XXII. Contaminated Immobilization Data onPolychlorinated Biphenyl 1248 Congenersfor Contaminated Dredged MaterialSolidified/Stabilized with 3 PercentPolymer and 20 Percent Portland Cement . . . 113

A-XXIII. Contaminant Immobilization Data onPolychlorinated Biphenyl 1248 Congenersfor Contaminated Dredged MaterialSolidified/Stabilized with 50 PercentFIRMEX ................... 114

xi

Table·

PageA-XXIV. Contamiuant Immobilizatiou Data ou

Polychlorinated Biphenyl 1248 Congeuersfor Contaminated Dredged MaterialSolidified/Stabilized with 3 Percent {Polymer and 50 Percent FIRMEX ....... 115

xii

LIST OF FIGURES

Figure Page1. Hypothetical Adsorption/Desorption Curve . . . 322. EPRI/Acurex Rotary Extractor (Tumbling

Apparatus) .................. 453. Comparison of Unconfined Compressive

Strength Between Portland Cement andPortland Cement with FIRMEX ......... 5l

4. Unconfined Compressive Strength of ThreePortland Cement Formulations ......... 52

5. Unconfined Compressive Strength of FIRMEXFormulations ................. 53

6. Unconfined Confined Strength of ThreePortland Cement and FIRMEX Formulations . . . 54

· 7. Unconfined Compressive Strength of ThreeWest—Paine Polymer Cement Formulations .... 55

8. Unconfined Compressive Strength of ThreeWest-Paine Polymer and FIRMEX Formulations . . 56

9. Histogram of the Average Aqueous PhaseConcentration of Arsenic at the LowestLiquid-Solids Ratio Versus Process Formula-tions .................... 65

10. Histogram of the Average Aqueous PhaseConcentration of Chromium at the Liquid-Solids Ratio with the Largest ConcentrationsVersus Process Formulations ......... 67

ll. Histogram of the Average Aqueous PhaseConcentration of Lead at the Lowest Liquid-Solids Ratio Versus Process Formulations . . . 68

12. Langmuir Isotherm of Contaminated DredgedMaterial Solidified with 60 Percent FIRMEX . . 7l

xiii

FigureA

Page13. Histogram of the Average Aqueous Phase

Concentration of Polyaromatic Hydrocarbonsat the Liquid—So1ids Ratio with theLargest Concentrations Versus ProcessFormulations ..................77

14. Histogram of the Average Aqueous PhaseConcentration of Polychlorinated Biphenyl1248 Congeners at the Liquid-Solids Ratiowith the Largest Concentrations VersusProcess Formulations ............. 78

15. Comparison of Process Formulations forNaphthalene Showing Low Aqueous PhaseConcentration at Low Liquid-Solids Ratios . . 80

xiv VA

Chapter 1. INTRODUCTION

Environmental protection has become a major concern ofthe public. This concern is embodied in various laws of the

W

United States that authorize protection of the environmentthrough regulation of waste disposal. Under Section 404 ofthe Clean Water Act and Section 103 of the Ocean Dumping Act,the Corps of Engineers (CE) was legislatively assigned theresponsibility of regulating transport and disposal ofdredged and fill material. Although the CE regulates dis-posal, the regulations are based on criteria developedjointly by the CE and the US Environmental Protection Agency(EPA) (1). Effective regulation involves a perspective thatrecognizes the interplay between past disposal practices thatwere inadequate, standard practices of today, and the re-

‘ search and development that is a necessary first step tofinding better alternatives.

In recent years, the management of bottom sediments

containing toxic substances has received increasing attention

from governmental agencies. Toxic substances are found insediments in industrial harbors and in waterways subject touncontrolled chemical releases and agricultural runoff.

Highly contaminated sediments can stress the aquatic_ ecosystem, resulting in reduced biological productivity and

bioaccumulation of contaminants in the food web (2,3,4,5).

]. .

42

When contaminated sediments are removed either for clean-upor maintenance of navigation channels, special controls maybe needed during dredging and disposal to minimize adverseenvironmental impacts. In certain situations, existing al-ternatives for disposal of highly contaminated sediment maylnot satisfy site-specific environmental constraints for dis-posal. If disposal of contaminated dredged material intosensitive environments is unavoidable, innovative contam-inant immobilization strategies may be needed.

The Corps of Engineers is responsible for the dredgingand disposal of large Volumes of sediment each year as partof its mission to improve, maintain, and extend navigablewaterways. Annual quantities of dredged material averageapproximately 290 million cubic meters in new work dredgingoperations (6). Over 90 percent of this dredged material isconsidered acceptable for a wide range of disposal alterna-tives (7). In addition to the CE dredging work, dredging isan alternatiVe·for remediation at Superfund sites involvingcontaminated sediments (8).

Three basic disposal alternatives for dredged materialare available (7):

a. Open-water disposal.

b. Confined disposal. (

c. Other (beneficial uses, etc.).‘

Confined disposal with restrictions is the alternative usu-ally considered the most appropriate for contaminated

, 3

sediments. A confined disposal facility (CDF) is a dikedarea for containment of dredged material. Dredged materialis usually placed in a CDF hydraulically by pipeline dredge,hopper dredge, or scow pumpout. Dredging of contaminatedsediment is occasionally restricted to mechanical dredging

~and placement of the material in a CDF by clamshell.

l

Contaminant migration follows several pathways from aCDF. These include release of contaminants in the effluentduring disposal of hydraulically dredged sediments, surface

· runoff of contaminants following disposal, leaching intogroundwater, plant and animal uptake directly from sediments,

animal uptake from feeding of plants, and volatilization ofcontaminants during and after placement of dredged material.To control or minimize potential environmental impacts, a CDFmust be designed and operated to contain dredged materialwithin the site and to restrict contaminant mobility. .

Present options for restricting contaminant mobility inV CDFs are limited to the use of liners, caps, and leachate

collection and treatment. Due to the volume of sediment in-volved 511 a typical dredging project (15,000 to 2 uüllioncubic meters), the cost of such systems can exceed the

available resources. In addition, these systems are not 100per cent effective. Hence, from a cost-benefit viewpoint,there is a need for less costly but equally effective alter-natives.

4

One promising contaminant immobilization technology issolidification/stabilization. Solidification/stabilizationis an emerging technology for producing stable solids withimproved contaminant isolation and containment character-

h istics of hazardous waste (9,10,11,12,13). Solidification/stabilization typically involves mixing setting agent(s) witha waste to form a hard, durable product that is substantiallyinsoluble in water and in which the waste contaminants areentrapped or micro-encapsulated in- the solidified mass(9,14).

4

The process of eliminating the free water in a semi-solid by hydration with a setting agent(s) is solidification.Stabilization is the physical and chemical alteration of thewaste to reduce contaminant mobility. Physical stabilizationrefers to improved geotechnical engineering properties suchas bearing capacity, trafficability, and improved environ-mental engineering properties such as reduced permeabilityand surface area for leachingI Chemical stabilization is the

alteration of the chemical form of the contaminants to makethem less soluble and/or less reactive. Solidification usu-ally* provides physical stabilization, but not necessarilychemical stabilization.

Since physical stabilization and solidification areequivalent in terms of the properties of the end product, theterms are often used interchangeably, with solidification

being the more commonly used term. The literature also uses

5

the terms "chemical stabilization" and "stabilization"interchangeably, albeit not without some confusion. In thismanuscript, physical stabilization and chemical stabiliza-tion are discussed together as solidification/stabilization

technology. The term "solidification/stabilization" refersto physical/chemical stabilization, unless otherwise noted.Where appropriate, contaminant immobilization ix; describedas primarily physical stabilization, chemical stabilization,

. or a combination of physical and chemical stabilization.

Several proprietary solidification systems are avail-able in the United States (9,15). Generic descriptions ofthese processes and a guide to their application has beenpublished by the Environmental Protection Agency (10). Mostof these processes are based on the use of the following

setting agents: portland cement, kiln dust, fly ash, lime,gypsum, and combinations of these materials. Co-additivessuch as bentonite, soluble silicates, and other materials aresometimes used with the setting agents to give special prop-erties to the final products. Patents have been issued for

-

some of the commercially available processes (US 4,184,958;US 4,079,003; US 4,028,240; US 4,149,968; US RE 29,783; US3,837,872), and additional patents may be pending.

6

OBJECTIVES

The overall objective of this study was to investigatethe technical feasibility of applying solidification/ sta-bilization technology to contaminated dredged material.Specific objectives were as follows:

a. Determine the physical strength of sediment after

solidification/stabilization processing

using various setting agents.

b. Determine the chemical leachability of sedimentafter solidification/stabilization processing

using various setting agents.

c. Investigate the relationship between physical· strength and chemical leachability.

d. Investigate the immobilization capability of a

proprietary polymer for selected organicl

contaminants when used in conjunction with

solidification/stabilization processes.

APPROACH

The research approach consisted of laboratory scale ap-plications of selected solidification/stabilization. proc-esses to Indiana Harbor sediment, and an evaluation of thesolidified/stabilized products on the basis of physical andchemical properties determined by laboratory testing.

CHAPTER 2. LITERATURE REVIEW

SOLIDIFICATION/STABILIZATION TECHNOLOGIES FOR HAZARDOUSWASTE

Solidification/stabilization is a relatively recent ap-

proach to the problem of containing hazardous waste. Some

of the early work included:

a. Mahloch et al (16), and involved several "fixation"

processes for hazardous industrial waste and flue

gas desulfurization sludges.

b. Mahloch (17), in an earlier paper, examined physi-

cal properties and leachability of chemicallyIstabilized hazardous waste.

c. Burk et al (18) researched the efficacy of polymer

impregnation of concrete solidified radioactive

waste. ·

These processes proved to be promising for containment of

hazardous waste and initiated continuing development of fur-

ther applications. A list of excellent references on current

solidification/stabilization technology is provided by

Tittlebaum et al. (9).

A large number of technologies are now available for the

solidification/stabilization of hazardous wastes. They have

as their goal the ultimate disposal of hazardous wastes. The

„ primary goal <xE hazardous waste treatment regardless of the

method used is to (10):

7

8

a. Improve the handling and physical characteristics

of the waste.

b. Decrease the surface area across which transfer or

loss of the contained pollutants can occur.

I bc. Limit the solubility of any pollutants contained

in the waste.

d. Detoxify contained pollutants.

Stabilization/solidification, processes have the potential

for achieving one or more of these goals (9).

Eight solidification/stabilization technologies are “

discussed in the literature. They can be grouped as follows

(9,10):

a. Solidification through the addition of cement.

b. Solidification through the addition of lime-based

or pozzolanic materials.

c. Treatment of the wastes to produce a cementitious

product without major additions of other products

(self-cementing).

d. Techniques involving embedding wastes in thermo-

plastic materials such as bitumen, paraffin or

polyethlene.

e. Solidification by addition of an organic polymer.

f. Encapsulation of wastes in an inert coating.

g. Formation of a glass or ceramic by fusion with

silica.

h. Miscellaneous processes.

9

Cement-Based Processes

Portland cement is the primary solidification reagent

in cement-based processes (9,10). It is added to waste or

sludge to create a solidified mass. Other materials may also

be added to the cement-sludge mixture, generally to lower the

cost associated with adding cement, such as fly ash cn: pro-i

prietary additives (19). Portland cement is a fused mixture

consisting of about 50% tricalcium and 25% dicalcium

silicates. Mixing* cement with water forms a colloidal

‘calcium—silicate-hydraue gel of indefinite composition and

structure. As the gel hydrates it forms silicate fibrils.

These interlocking fibrils bind the cement and various hy-

dration products into the hardening mass (20,21). The hard-

ened product produced has a relatively high bearing capacity.

Use of cementation is especially effective with toxic

metals. The cement mixture creates a mixture with a high pH;

most multivalent cations are converted into insoluble

hydroxides or carbonates. Metal ions may also be incorpo-

rated into the crystal structure of the cement minerals that

form (10).

Leaching studies have shown that without pretreatment

organics will leach out of the mass (22). Immobilization of

organic compounds, using cement-based processes, has not been

successfully demonstrated. In an EPA study of kepone in theJames River, it was shown that elevated pH increased solu-

bility of kepone in the sediment (23,24).

].O

Certain inorganic and organic compounds interfere with

the setting and curing of the cement-sludge, such as: oil

and grease, phenol, sulfates, strong bases, pesticides,

lignite, degreasers, and salts of copper, lead, and zinc.

A Calcium hydroxide is also reported to retard the cement-

setting process (10,25).

Advantages and disadvantages of the cement-based process

are listed in Table I. ,

Lime-based and Pozzolanic Processes

Also cementitious are lime-based and pozzolanic process

(9,10) which depend on a reaction of lime with a fine-grained

siliceous (pozzolanic) material and water. Most common

pozzolanic materials used include fly ash, ground blast fur-

nace slag, and cement kiln dust. These materials are not

always pozzolanic but must be tested for each case to deter-

mine cementaceous properties. Many pozzolanic materials have

been patented by manufacturers and marketed as hazardous

waste fixatives. FIRMEX ix; one such proprietary material.

Characteristics of lime-based and pozzolanic processes are

similar to cement-based process. Advantages and disadvan-

tages of the lime-based and pozzolanic processes are shown

in Table II.

ll

TABLE I. ADVANTAGES AND DISADVANTAGES OF CEMENT-BASE PROCESS (10)

Advantages:

The amount of cement used can be varied to produce high bearing.capacities (making the waste concrete good subgrade and sub-foundation materials) and low permeability in the product.

Raw materials are plentiful and inexpensive.

The technology and management of cement mixing and handling is wellknown, the equipment is commonplace, and specialized labor is notrequired.

Extensive drying or dewatering of waste is not required becausecement mixtures require water, and the amount of cement added canbe adapted through wide ranges of water contents.

The system is tolerant of most chemical Variations. The naturalalkalinity of the cement used can neutralize acids. Cement is notaffected by strong oxidizers such as nitrates or chlorates. Pre-treatment is required only for materials that retard or interferewith the setting action of cement.

Leaching characteristics can be improved where necessary by coatingthe resulting product with a sealant.

Disadvantages:

Relatively large amounts of cement are required for most treatmentprocesses (but this may partly be offset by the low cost ofmaterial). The weight and Volue of the final product istypically about double those of other solidification processes. _

Uncoated cement-based products may require a well-designed land-fill for burial. Experience in radioactive waste disposal indi-cates that some wastes are leached from the solidified concrete,especially by mildly acidic leaching solutions.

Extensive pretreatment, more expensive cement types or additivesmay be necessary for waste containing large amounts of impuritiessuch as borates and sulfates that affect the setting or curing ofthe waste—concrete mixture.

The alkalinity of cement drives off ammonium ion as ammonia gas.

Cement is an energy-intensive material.

I2

TABLE II. ADVANTAGES AND DISADVANTAGES OF LIME—BASED

AND POZZOLANIC PROCESSES (10)

Advantages:

Product is generally a solid with improved handling and permeabi-lity characteristics.

The materials are often very low in cost and widely available.

Little specialized equipment is required for processing, as limeis a common additive in other waste streams.

The chemistry of lime—pozzolanic reactions are relatively well-known. Sulfate does not cause spalling or cracking.

Extensive dewatering is not necessary because water is requiredin the setting reaction.

Disadvantages: VLime and other additives add to the weight and bulk to be trans-ported and/or landfilled.

Uncoated lime-treated materials may require specially designedlandfills to guarantee that the material does not lose potentialpollutants by leaching.

l13

Self-cementing Process

Se1f—cementing properties (9,10) in waste can be createdusing flue gas cleaning and desulfurization sludges with

proprietary additives. Large amounts of calcium sulfite or

calcium sulfate are contained in these sludges. A smallportion of the waste, eight to ten percent, which has been

dewatered is calcined to produce a partially dehydratedcementitious calcium sulfate or sulfite. The calcined prod-uct is reintroduced to the waste sludge to produce a hard

plaster-like material with good handling characteristics.

Thermoplastic Technique

The thermoplastic technique (9,10) was originally de-

veloped for containment of radioactive waste but has the po-

tential for adaptation to industrial waste. A plastic

matrix, normally consisting of bitumen, paraffin, or

polyethylene, is initially heated to 180°CZ to 230°C. Haz-

ardous waste which has been dried is then heated and dis-persed through the plastic matrix. After combining, the

mixture is cooled to solidify the mass and usually placed

into a secondary containment system such as a steel drum.

Specialized equipment and training is required for processing

as opposed to cement-based and pozzolanic processes. Ratio

of matrix to waste is quite large, usually 1:1 to 1:2. The3

matrix material is also quite expensive. However, the rate

of loss to contacting fluids is significantly lower than

14

those observed with cement—based. and pozzolanic process.Major drawbacks to this process include the fact that thewaste must be dry. Organic chemicals that are solvents forthe matrix material obviously cannot be used. Strong

oxidizer also creates problems especially fires and dehy-

drated salts rehydrate when soaked in water which cause the

matrix to split open.

Organic Polymer Process

Organic polymer processing was originally developed for

transportation of hazardous waste (9,10). Urea formaldehyde

is the most commonly used polymer. Dewatered waste is mixed

with prepolymer. Catalyst is then added and mixed thor-

oughly. Before forming a resin the mixture is poured into a

waste container. The final product is a spongy mass which

contains the waste that generally must be dried. No chemical

reactions occur in the solidification process that binds the

contaminants; therefore, leaching can occur more readily than

with cement-based processes. Mixing and setting of the resinmust take place at low pH values. Toxic metals are known tosolubilize and leach out at low pH. When. drying thepolymerized waste will "weep" concentrated acids and toxic

pollutants. Toxic fumes are also associated vnJü1 aging

polymerized waste.

15

Encapsulation Jacketing

Encapsulation processes have been developed to handletoxic wastes not adequately contained by other processes(9,10). The processes previously described also encapsulateby coating the waste material. Encapsulation takes the con-tainment of hazardous waste one step further. Hazardous

U

waste, which can. be also previously solidified kur otherprocesses, is coated in an inert material such as:polyethylene, polybutadiene, polyurethane, and fiberglassepoxides. Highly* soluble wastes can. be contained. whicheliminates leaching, however, it is impractical for use withlarge quantities of waste.

i

Glass and Ceramic Processes

Glass and ceramic processes are restricted to use incontainment of radioactive wastes and therefore are beyondthe scope of this manuscript.

Other Processes

Other processes include:

a. Polyfilla——a plaster and cellulose material addedto contaminated soils and organic solvents (9,10).

b. ARDECCA——a proprietary material with fly ash used

to handle oilfield wastes (9,10).

c. Ansorb--a clay deposit product used for both liquid

and dewatered wastes (9,10).

16

Waterways Experiment Station has experimented with

sorbent assisted solidification using organosilanes to en-hance adsorption of soils for containment of wastes (26).

There are obviously many various technologies and mod-

, ifications for solidification/stabilization of wastes. They

handle a whole range of wastes and no process is applicable

to every waste. The amount and type of waste along with the

economics and the type of disposal site are important factors

in selecting a solidification/stabilization technology.

SOLIDIFICATION/STABILIZATION TECHNOLOGIES FOR DREDGEDMATERIAL _Solidification/stabilization of dredged material is

unique because of the volume of material which must be proc-

essed. Most of the technologies previously mentioned deal

in terms of pounds, kilograms or liters of contaminated

waste. Dredge material must be processed in quantities of

cubic meters, cubic yards, or tons of material.Cement-based and pozzolanic-based. processes predomi-

nantly have been the techniques used to solidify/stabilize

both clean and contaminated sediments (22,27). The majorityof published work on solidification/stabilization. of

sediments has been done by the Japanese

(29,30,3l,32,33,34,35). Most of the Japanese work has been

oriented toward processing sediment into reclaimable land

(physical stabilization). For this reason there has been

17

more emphasis on construction than on environment aspects.U. S. research has focused more effort on environmental ap-plications to solidify/stabilize contaminated dredge mate-rial (11,28,36).

Japanese Studies

Kita and Kubo_ (29) reported that the softness ofsediments create a great obstacle to work especially whenhauling of dredged sediment to containment areas. The au-

thors define stabilization as being divided into three cate-

gories: sun drying, consolidation drainage, andsolidification. Solidification. is preferred because

sediments can be stabilized in a shorter time and to a higher

strength. Four techniques for solidification of sedimentsare proposed. Cement-based and pozzolanic additives are usedin all four techniques. Kita and Kubo also reported fourfactors that influence the strength of solidified sediments:

a. properties of the bottom sediment (i.e. water con-tent, grain size distribution and organic content).

b. the type, combination and quantity of solidificants.c. sediment and solidificant mixing condition.

d. curing temperature and time.

Kamon (30) used lime-cement with aluminum sulfate as asolidificant to stabilize soft freshwater clay.

Murakami (31) reported on. the results of full-scale

solidification treatment of organically polluted mud from the

18 .

Seto Inland Sea in Japan. The bottom mud was dredged and thentransferred to sedimentation pontoons. Treatment by coag-ulation and sedimentation was followed by dehydration.’ Theresulting settled sludge was hardened by mixing with cementand placed cux a reserved land area and then covered withsand.

Okumura (32) stated that cement-based and lime stabili-zation is the most frequently used solidificants. He re-ported unconfined compressive strengths that reached 327 psiin several marine sediments.

° Oshita (33) reported on the results of a new method oftreating bottom sediments, the SIL—B treatment method. Asilicic coagulant called Siloxy—silanol or siloxane is mixedwith bottom sediments to produce a highly hydrous sedimentreferred to as a hydrogel. The fixed sediment has a very weakbearing capacity, however, and the sediment hydrates quickly.It was proposed that siloxane may be useful in containingtoxic metals because it has the advantage of maintaining aneutral pH as opposed to cement-based and lime-basedsolidificants. Sil-B treatment method was used to stabilizeapproximately 362,000 cubic yards of contaminated. bottomsediment in the River Waka in Japan. Sediment was mixed in-situ and dredged up after hardening. Tabuse (35) reported

.that there were no metals leached from the sediment. It wasalso reported that sediment Volume was reduced by fifty per-cent.

].9

Otsuki and Shima (34), using a seawater to cement ratioof sixty percent, reported unconfined compressive strengths

between 809 and 1072 psi after three months of

solidification.

U. S. Studies

In the United States, stabilization techniques are used

almost exclusively in oil and gas drilling operations and onwastes from power plants, chemical manufacturing, and thenuclear industry as opposed to the Japanese who use the ‘

techniques for improving handling and bearing capacity of

sediments (ll). Of thirty-three cases of contaminated

sediments remediation in the U.S., only in two cases, the

Upper Hudson. River· in. New 'York, and. Waukegan. Harbor in

Illinois, was stabilization considered. To date there areno actual cases where the technique has been used in the U.S.

(ll).

Krizek et al (36) reported on the results of lime addi-

tion to dredged material and its effects on pollution poten-

tial. A reduction in pollution potential was found and theresulting leachates were not a potentially serious hazard.

Francingues (11) described two goals of stabilization· and solidification with respect to dredge material. Sta-

bilization systems attempt to reduce the solubility or reac-tivity of a waste. Solidification systems attempt to convertthe waste into an easily handleable solid with reduced hazard

20

from leaching or spillage. Three implementation strategies

were proposed:

a. In situ mixing involves introducing sorbents or

solidificants directly into the contaminated sedi-

ment and mixing in place. The sediment can then

either be covered in place or removed after solidi-

fication.

b. Plant mixing requires removal of contaminated sedi-

ment and mixing of solidificants or sorbents in a

batch plant then movement to a disposal area.

. c. Area mixing is the third proposed strategy. Hori-lzontal construction equipment is used to add and

‘ mix solidificants or sorbents.

Ludwig et al (28) proposed four strategies to implement

solidification/stabilization technology for improved manage-

ment and disposal of contaminated dredged material. The

strategies described are confined disposal facility (CDF)

physical solidification, CDF chemical solidification,

aquatic disposal and chemically solidified upland disposal.

TEST PROCEDURES FOR PHYSICAL-CHEMICAL EVALUATION OFSOLIDIFIED/STABILIZED PRODUCTS

Solidified/stabilized products vary in physical-

chemical characteristics depending on the waste, the process

additives, and the formulation used. The state-of-the-artd

is such that a solidification/stabilization process cannot

2l '

{be formulated on the basis of waste characteristics alone.It is therefore necessary to conduct physical-chemical prop-erties testing to properly evaluate the effectiveness ofsolidification/stabilization for a specific waste orsediment. In addition, certain waste constituents can in-terfere with the setting reactions responsible for develop-ment of a hardened mass (25). Thus, vendors usually develop

_ a process formulation for aa specific waste. For another2waste with similar characteristics, the process formulationmay be different.

In the review that follows, various laboratory tests fordetermining the physical-chemical properties ofsolidified/stabilized products are discussed„ A review oftest procedures is necessary because there are no standard-ized laboratory protocols for evaluating the suitability ofsolidified/stabilized waste or dredged material for disposal.

Physical Properties

Physical stabilization (solidification) immobilizes’ contaminants through alteration of the physical character of

the material. The development of structure immobilizes con-taminated solids, i.e., the solid mass is dimensionally sta-ble, and the solids do not move. Since most of thecontaminants in dredged material are tightly bound txa thesediment phase, solidification is an important contaminantimmobilizing mechanism (29). Solidification also reduces the

22

-accessibility of water to the contaminated solids within acemented nmtrix. Water accessibility to the contaminated

solid is an important factor because it partially determines

the rate at which contaminants are leached.

Bartos and Palmero (37), in their pioneering work on the

engineering properties of solidified/stabilized sludges,

conducted five different tests that are normally used in

soils testing. These tests along with references on the

procedures are listed in Table III. A brief description of

the information provided by each of the five basic tests

follows. Bulk and dry unit weight can be used to compute

overburden pressure. Unconfined compressive strength is an

important factor in determining ultimate bearing capacity,

stability of embankments, and, pressure- against retaining

- walls. Permeability is an important parameter because it

partly determines the rate at which contaminants can be re-

leased kwr chemical leaching. Wet/dry durability testing

provides information on the resistance of solidified products1 to the natural weathering stresses of wetting and drying and

the freeze-thaw durability test provides information on the

resistance of solidified/stabilized products to the natural

weathering stresses of freezing and thawing.

Bartos and Palmero's battery of tests and procedures has

been, until recently, the standard for developing information

on the durability and long-term physical characteristic of

solidified/stabilizad wastes (10,15). Unconfined/confined

23

TABLE III. STANDARD TESTS FOR PHYSICAL PROPERTIES OF SOILSl

Test Reference

Bulk and dry unit weight Appendix II of EM lllO—2-l906

Unconfined compressive strength ASTM method D2l66—66

Permeabilityl

Appendix VII of EM lllO-2-1906

Wet/dry durability ASTM method D559—57

Freeze/thaw durability ASTM method D560—57

Y 24

compressive strength procedures used by Bartos and Palmero

is a soils test (ASTM D2166) that involves the preparation

and testing of a cylinder. ASTM test for unconfined

compressive strength of hydraulic cement mortar (ASTM C-109)

has replaced this test. This hydraulic mortar test involves

the preparation and testing of 2 inch (5 cm) cubes. Test

procedure for unconfined compressive strength was changed

because the cement mortar procedure is more reproducible than

the soils procedure and because freshly prepared

solidified/stabilized material resemblesfresh mortar more

than it resembles soil (38). Other tests that are sometimes

run include solids specific gravity and porosity.

Porosity is aui important factor in determining the ac-

cessibility of water to the contaminated solids. If contam-

inant transport is principally diffusion controlled transport

from inside the voids out to exposed surfaces, then porosity

may be more indicative of leaching “potential than

permeability. A standard procedure for solidified/stabilized

waste is under development by ASTM (Hannak, 1985) (39).

Bartos and IPa1ermo (37) also determined porosity, but a

standard soils procedure was not used because specific pro-

cedures for solidified/stabilized waste were not available.

It is possible that an improved. method for determining

porosity will be developed specifically forsolidified/stabilized materials and that this parameter will

25

become part of the standard list of physical properties teststo conduct.

There are little published data on the physical proper-ties of solidified/stabilized waste, other than that reported

by Bartos and Palermo (37). These data show

solidified/stabilized waste with unconfined compressive

strength i11 a range comparable with stiff clay to soft con-

crete (20 to 2000 psi). Table IV provides a summary of un-

confined compressive strengths for various materials.

Permeability was in the range normally associated with silts

to tight clays (l0E—05 to l0E-ll cm/sec).

There are no criteria or guidelines to compare with

laboratory data generated on physical properties. The lim-

ited data on the physical properties of solidified/stabilized

materials, the lack of long-term records on solidified waste

landfills, and absence of a clear connection between impor-

tant physical properties such as unconfined compressive

strength with chemical leachability have apparently hindered'

the development of meaningful criteria by regulatory agen-

cies. Without criteria, potential users and permit writers

alike don't know how 1u> evaluate proposed solidification,

landfill projects. Thus, the absence of accepted criteria

- for field performance has been a major obstacle to implemen-

tation of this technology. (

26

TABLE IV. UNCOMFINED COMRESSIVE STRENGTHS OF VARIOUS MATERIALS

UnconfinedCompressiveStrength

Material Type (psi)

Clay (40) Very soft < 3.5Soft 3.5-7Medium 7-14Stiff 14-28Hard 28-56nVery hard ·> 56

Solid-like FGD sludge 23-43solidified waste (37) Electroplating sludge 32u

NI/CD battery sludge 8Brine sludge 22CA fluoride sludge 25

Cement—based (10) Flue gas cleaning waste 2570

Lime—based pozzolan NI/CD battery sludge 169Vproduct (10) Electroplating sludge 77

Chlorine production waste 133

Concrete Low strength 2000Medium strength 5000

27

Leachability

A description of the testing procedures for leachabilityis more varied than that for physical properties. The firstcomprehensive review of leaching test methods was providedby Lowenbach (4l). Lowenbach reported testing variables suchas pH, test duration, liquid-to-solids ratio, sample prepa-ration, and, method of agitation for 30 leaching tests.

. Lowenbach also presented mass transport theory for inter-preting leach tests. The majority of the leaching testscompiled were designed, however, on the basis of arbitraryassumptions regarding the testing variables listed above andnot on the basis of mass transport theory., Hence, the testprocedures did not supply the type of information suitablefor application of mass transport theory to the field situ-ation. Only one of the leach procedures reported byLowenbach was designed around mass transport theory. Thiswas the test used by the International Atomic Energy Agency

‘i (IAEA) to leach solidified/stabilized radioactive waste (42).As a consequence, a wide variety of laboratory leach testswere available for non-radioactive waste for which there wasno way of extrapolating the data to predict field leachate

quality.

Since Lowenbach's report there have been three volumes

on hazardous waste testing that include descriptions andcriticisms of laboratory leaching tests published by theAmerican Society_for Testing and Materials (43,44,45). In

28

the first volume, Perket and Webster ‘(46) provide achronology of the major developments leading· up to thestandard leaching ‘test for hazardous waste, the EPA Ex-

traction Procedure (EP) (47). The EP has been criticized inall three Volumes and in particular, by Lee and Jones (48).

The EPA Extraction Procedure is a criteria—comparisontype test in which results from a standardized procedure arecompared to a specific set of concentration limits. If anyone of fourteen pollutant concentrations in the EP leachateare equal to or greater than the published limit, thesolidified waste has failed the EP. Materials that fail theEP are regulatorily defined as hazardous. The test consistsof contacting dilute acetic acid with approximately 100 grams

of solidified waste in a liquid to solids ratio that variesbetween 16:1 to 20:1 depending on waste alkalinity. The du-ration of the test varies from 24 to 28 hours, also dependingon waste alkalinity.

Because the EP test results do not provide informationon leaching kinetics, equilibrium coefficients, or mass

transfer coefficients, the data are not suitable for umsstransport equations (49). The utility of the EP as a labo-

ratory scale simulation of dredged material disposal is also

limited. In particular, the leachant pH, oxidation—reduction

potential, and the liquid—solids ratio used in the EP do notsimulate field conditions for dredged material disposal. The

geochemistry of dredged material is not properly simulated

29

in the test, and studies have shown that the EP is a poorpredictor of the leachate quality associated to contaminatedsediments (19).

In the third ASTM volume, Cote and Isabel (50) de-

scribed a leaching test for solidified/stabilized waste thatis a modification of the procedure described by Hespe (42)and later by Malone, Jones, and Larson (10). The procedureinvolves suspending a cylinder of solidified/stabilized wastein a leachant (i.e. distilled-deionized water) that is peri-odically renewed. Each time the leachant is renewed, thereplaced leachate is analyzed for soluble contaminants. Theappearance of contaminant in the leachate, expressed as theaccumulated fraction of contaminant originally in the speci-men at the beginning of the test, is plotted as a function

‘ of the square root of time. If the rate of appearance of

contaminant in the leachate is controlled by diffusionfromwithinthe specimen to the surfaces that are leached, the

plot will result in a straight line. From the slope of thisline an intrinsic parameter that characterizes theleachability, effective diffusivity, can be calculated.Given that all the attendant assumptions and boundary andlinitial conditions are satisfied, effective diffusivity canbe used to calculate the field contaminant immobilizatidn

provided by solidification/stabilization of a waste.Diffusion controlled transport of contaminant to sur-

faC&S of a mOr10lith basically ignores convection. The Cote

30

and Isabel model best applies to impermeable waste that arewell isolated from the hydrologic cycle (51). An alternativemigration. pathway is via infiltration of water· into ·thesolidified waste, leaching ·of contaminants from the

solidified waste as this water percolates through the land-fill, and then movement of a leachate generated by thisprocess into the environment. Permeant-porous media proc-esses are modeled with an advection-diffusion equation thatincludes a source term that describes contaminant transferfrom the solid phase to the aqueous phase (41,52,53,54). Touse a permeant-porous media model, laboratory procedures areneeded to define the source term in the mathematical formsuitale for inclusion i11 an advection-dispersion equationwith reaction. Standard procedures applicable tosolidified/stabilized waste are not available for this pur-pose.

-‘

Hill, Myers, and Brannon (49) reviewed procedures fordetermining the source term for untreated dredged material

and recommended for study a model that describes contaminanttransfer from the dredged material solids to the aqueousphase as equilibrium controlled desorption. In the equilib-rium controlled desorption approach, solid phase contaminantconcentration and aqueous phase contaminent concentration arerelated by a single distribution coefficient. This distrib-ution coefficient. is determined by plotting a desorption

isotherm. A theoretical desorption isothemn is shown in

31

Figure 1. Data for plotting a desorption isotherm are ob-

tained by sequentially leaching a sample of dredged material

and analyzing the soluble contaminant concentrations after

each step in the leaching sequence. From the data obtained,

solid phase concentration and aqueous phase concentration can

be determined and Figures plotted.

The distribution coefficient is the slope of the

desorption isotherm. The larger time distribution coeffi-

cient, the lower the aqueous phase concentration that a given

solid phase concentration will support. If the desorption

isotherm intercepts the ordinate, the intercept represents a

leaching resistant fraction of the solid phase concentration.n

The equilibrium controlled desorption model adequately

describes reversible processes such as sorption of organics

and ion-exchange of inorganics (54). Not taken into account

is changing leachant chemistry, nor does it model leaching

of solubility limited contaminants. Alternative models for 'transfer of contaminants from the dredged material solids to·

the aqueous phase have been described by Hill, Myers, and

Brannon (49). The equilibrium controlled desorption model

has not been verified for either untreatmd or solidified

dredged material; however, it has been used to model leaching‘ of contaminated soils (52,53,54).

A modification to the sequential leaching approach to

generating a desorption isotherm is the serial leach proce-

dure described by Houle and Long (55). In the serial leach

32

¤·ZQP

•

<cc .}- 1zLU0ä “ ~0 ' OÜ

p,?1‘< €gO{ _ 0•-

.E \Q‘x¤ . ’xä es. SO

0· Y

¢ e

AQUEOUS PHASE CONCENTRATION, C

”Figure l. Theoretical adsorption/desorpciou isocherm (25).

33

procedure, a sample is leached one time at several liquid-solid ratios. Again solid phase and aqueous phase concen-

trations are edetermined. and. Figures plotted. Laboratory

application of this procedure is easier. In.applying this

procedure, it is assumed that the liquid-solid ratio does not

affect the chemistry of the leaching process. Serial, graded

batch leach procedures have been used to construct desorption. isotherms for a solidified/stabilized hazardous waste (25).3

The serial batch leach procedure also assumes that the

liquid—solids ratio does not affect the chemistry of the

leaching process, i.e., the distribution coefficient is not

dependent on liquid-solids ratio. Literature indicates that

this assumption is probably not correct for untreated

sediment, although the reason for this is not entirely clear(56). For sediment: that. has been solidified/stabilized,

changes in the chemistry of the aqueous phase with varying

liquid-solids ratio probably have a more profound effect on

the distribution coefficient than changes in the concen-

tration of solids. Specifically, if pH varies significantly,

the solubility of metals may vary. However, the constituents

in the solidification reagents tend to stabilize pH (19).

CHAPTER 3. MATERIALS AND METHODS

The purpose of this research was to apply state-of-the-art technology for solidification/stabilization to contam-inated dredge material in a laboratory study. Contaminateddredged material was taken from the heavily polluted IndianaHarbor Canal, at its junction with Lake Michigan near Gary,

IN. Primary use of this canal is to provide commercial ‘

shipping access to industrial sites located along the canalwhose flow is estimated to be 50 percent industrial effluents(26). The Army Corps of Engineers, Chicago District, is ·

proposing to dredge approximately 200,000 cubic yards ofsediment to maintain authorized depth in the canal. Approx-imately 50,000 cubic yards of this sediment has been classi-fied as toxic, as i€?exceeds the EPA standards of 50 ppb PCBsfor sediments (26h; Analysis of Table V reveals the seriouscondition of canal sediment in comparison with average LakeMichigan sediments.

MATERIALS

Sediment samples were collected by the Waterways Exper-

iment Station using a clamshell dredge at a sediment depthof five to six feet. A dredge was hoisted above a 55-gallon

clean steel drum, the bucket opened and a portion of thesediment was allowed to drop into the drum. Twenty-fivedrums were collected.

_ 34

35

TABLE V. COMTARAIIVE CHEMICAL COMPOSITION OF INDIANA HARBORAND LAKE MICHIGAN SEDIMENTS (26)

Concentration in Sediment (mg/kg Dry Wt.)Parameter Indiana Harbor Lake Michigan

MetalsArsenic 29.5 10.1Cadmium 20.0 0.1Chromium 282.0 4.4Copper 266.0 ·-—Iron 182000 -·Lead 879.0 11.9Manganese 2085 ·—·Mercury 0.5 BD*Nickel 120.0 —-—Zinc 4125.0 54.1

PesticidesAldrin 2.55 0.0006Polyaromatic Hydrocarbons (PAH's)

Acenapthene 96 BDAcenapthylene 22 BDAnthracene 62 BDBenzo(a)anthracene 86 BDBenzo(b)f1uoranthene 140 BDBe¤zo(a)pyre¤e 87 _ BDBenzo(G H I)pery1ene 35 BDChrysene 92 BDFluoranthene 150 BDFluorene 69 BDIndeno(l,2,3-C D)pyrene 50 BDNaphthalene 2000 0.46Phenanthrene 200 BD‘ Pyrene 140 BD

Polychlorinated Biphenyls (PCB's)PCB—l248 127.*8 BDPCB-1254 BD 0.013Total Organic Carbon 24000 (12.52 of 1700 (1.832 of

sediment weight) sediment weight)

Total Inorganic Carbon 211 (1.12 of . 438 (0.472 ofsediment weight) sediment weight)

Oil and Grease 11000 (5.12 of 1586 (1.712 ofsediment weight) sediment weight)

Phenol 3 BD

*BD — below detection

364

The drums were then sealed and transported in a refrig-erated truck to Waterways Experiment Station . Upon arrival,the sediment was homogenized using a clean concrete mixer andreturned to 55·gallon steel drums then stored at 4°C untilused. Contents of the sediment container (55-gal drum) weremixed again, prior to solidification, using a 3 h.p. motorwith a stainless steel mixing blade. No processing (e.g.dewatering) was undertaken prior to application of the vari-ous processes. Solidification/stabilization materials in-cluded:

a. Type I Portland cement, used in the processes in-volving Portland cement.

b. FIRMEX, a proprietary additive, is a solidifica—tion agent that is commercially available. FIRMEXwas obtained from Trident Engineering, Baltimore,MD.

··

c. A proprietary polymer, WEST-PAINE polymer (57), was’ obtained from Philip W. West, retired Professor of

Chemistry, Louisiana State University. The polymeris still in the research and testing stage ofdevelopment and was not commercially available atthe time this research was conducted.

37 '

EXPERIMENTAL DESIGN

Laboratory‘ scale application of solidification/ sta-bilization technology to contaminated Indiana Harbor dredgedmaterial was examined for both physical and chemical sta-bilization. Physical stabilization was evaluated kur deter-mining unconfined compressive strength, whereas chemicalstabilization was evaluated by running serial batch leachingtests.

Cement-based and pozzolanic-based technologies wereused in this research to convert contaminated sediment intoa solidified product. Polymer was added to various processformulations to determine effect on organic leaching. Proc-_ess formulations (mix ratios) used in this research are shownin Tables VI and VII. .

Each process was applied in three mix ratios except forPortland cement which was applied in four mix ratios. For-mulations for each process differed with respect to dosageof setting agent used, not by type of agent used. By testing •

.

different processes in varying strengths, data were obtainedfor making comparisons among processes and process mix ra-tios. Screening evaluations were conducted by the WaterwaysExperiment Station along with advice from sources providing

. proprietary materials (57) to determine which process andprocess mix ratios to use.

38

TABLE VI. SOLIDIFICATIONXSTABILIZATION PROCESS MIX RATIOSA

Ratios, by Percent Weight of MaterialProcess (Sedimentzlst Materia1:2nd Material)

A. Portland cement 1:0.1, 1:0.2, 1:0.3, 1:0.4

B. Portland cement:FIRMEX 1:0.2:0.1, 1:0.1:0.2, 1:0.15:0.15

C. Portland cementzpolymer 1:0.2:0.1, 1:0.2:0.3, 1:0.2:0.05

D. FIRMEX 1:0.4, 1:0.5, 1:0.6

E. FIRHEX:po1ymer 1:0.5:0.0l, 1:0.5:0.03, 1:0.5:0.05

39

TABLE VII. PROCESS MIX RATIOS FOR SERIAL, GRADED BATCH LEACHING TESTOF PAHS AND PCB CONGENERS

Ratios by Percent Weight of MaterialProcess (Sedimentzlst Materia1:2nd Material)

Portland cement 1:0.2

Portland cementzpolymer 1:0.2:0.03

FIRMEX « 1:0.5

FIRMEX:po1ymer 1:0.5:0.03

40 ‘

LABORATORY PROCEDURE

Sample Processing

A mixed sediment sample was removed from az sealed con-tainer and weighed on a Beckman 3000 scale. The sediment wastransferred to a Hobart C-100 mixer. Additives were thenweighed and added to the mixer which was operated for ap-proximately five minutes at low speed. After mixing, thefreshly prepared solidified sediment was poured into 2—inch(5.1 cm) brass cube molds and standard 4-inch CE compactionmolds. The molds had been prepared with a light coating of _

mold grease to facilitate removal of the solidified sediment.The molds were shaken on a vibrating table to eliminatevoids, as freshly prepared solidified sediment was placedinto the molds with a spatula.

4Approximate1y 24 hours after pouring the molds, (EIRMEXand FIRMEX with.polymer, 48 hours), the sediment was removed.Samples were cured at 98% relative humidity and 23°C untiltested. A standard cure time- of 28 days was used unlessotherwise noted.

Unconfined Compressive Strength Testing

Unconfined compressive strengths were determined in ac-cordance with the ASTM Compressive Strength of Hydraulic Ce-ment Mortars (C-109) procedure. Testing* intervals wereinitially established at 7, 14, 21, and 28 days for Portland

41

cement. When testing of FIRMEX samples began it was decidedto increase testing to 60 and 90 days in addition 1x> thepreviously described intervals. Rationale for this decisionis provided i11 the discussion section of Chapter 4. Threereplicate samples were tested at each interval except thatsix replicates were tested for Portland cement at 14 and 28days. Six replicates were not used in the other processesbecause available facilities precluded the storage of a largenumber of samples needed for 90 days. Two-inch sample cubesin the numbers required were removed from the curing chamberat the intervals indicated. Dimensions were measured with acaliper and recorded. Sample cubes were placed into plasticZiploc bags to prevent contamination of the work area priorto testing. (Note: Testing had previously been conductedto show that placement in the plastic bags had no effect onstrength.) The cubes were then tested with a hydraulic pressthat determines gauge strength electronically. Gauge

strength was converted to pounds per square inch (psi) bydividing gauge strength by total area of the cube.

Serial Batch Leach Testing for Metals and Total Organic Car-@1Chemical leach tests were conducted <x1 samples taken

from the center of the 4-inch cylinder samples cast in com-paction molds. The 4-inch samples first had the outside 1/4inch removed with a clean stainless steel scraper to elimi-

42

nate contamination from mold grease. The samples were thenbroken apart and dried for 24 hours under a ventilation hood.After 24 hours, the samples were ground in a Brinkmancentrifugal grindingmill to pass a 0.5 mm screen beforeleach testing. The leach procedure consisted of contactingground solidified sediment samples with distilled—deionizedwater one time (55) on an Eberbach mechanical shaker on lowspeed for 24 hours in the following liquid-solids ratios:100 ml:50 g, 100 ml:20 g, 100 ml:10 g, 100 ml:5 g, and 100m1:1 g. In the Portland cement formulations, the 100 ml:20g liquid-solids ratio was not used. It was determined afterthe Portland cement formulations were tested that the extradata would improve the reliability of information obtainedby curve fitting. The liquid-solids ratios were run intriplicate and placed into 250 ml Nalgene polyethylene bot-tles laid on their sides. This resulted in fifteen bottlesplus a blank for extraction. After shaking, the mixtureswere filtered through Type HA 0.45 mm Millipore filters, withstandard, acid washed, plastic Millipore filtration apparatuswith vacuum pump assistance. After filtration, the filtratewas placed into 125 ml Nalgene polyethylene bottles. Samplesto be tested for metals and arsenic were preserved with 250ul ultrex nitric acid. Samples to be tested for total or-

ganic carbon were preserved with 250 ul concentrated HZSO,Analysis was conducted to determine the presence of:arsenic, cadmium, chromium, lead, zinc, and total organic

434

carbon in the leachate. The preserved samples were turnedinto the Analytical Laboratory Group for analysis. Chemicalanalysis procedures used are found in the following section.

Serial Batch Leach Testing for Polyaromatic Hydrocarbons andPolychlorinated Biphenyl Congeners

A modification of the leach procedure, previously de-scribed, was conducted for analysis of' polyaromatichydrocarbons (PAHs) and polychlorinated biphenyl (PCB) 1248congeners. Four different formulations were prepared to de-termine the effectiveness of West-Paine polymer with cementbased or pozzolanic—based formulations in preventing leachingof organics, specifically PCBs. Formulations tested

lare

shown in Table VII. Sediment was prepared and poured into4-inch compaction molds and allowed to cure as pmeviouslydescribed„ At 21 days, 4-inch cylinders were processed aspreviously described. The procedure for leaching consistedof contacting solidified sediment samples with distilled-deionized water for 24 hours in the following liquid—solidsratios: 1000 ml:500 g, 1000 ml:200 g, 1000 ml:100 g, 1000

ml:50 g, and 1000 ml:10 g. Samples were then placed into new

one-half gallon glass containers that were acetone washed.

Lids for the containers were polyethylene lined and alsoacetone washad. Five containers per formulation and one

blank per formulation were prepared. The containers werethen tumbled at 32 r.p.m. for 24 hrs in EPRI/Acurex Rotary

l44

4

Extractor, a tumbling apparatus such as depicted in Figure 2(47). After tumbling, the samples were allowed to settle forabout one hour, after which sample leachate was filtered us-ing aa type A/E 47 mm Gelman glass filter. Filter apparatus

l

consisted of an acetone washed, glass, Vacuum, Milliporefilter system. Filtered leachate was then. placed intoacetone-washed one—half gallon containers and turned into ALGfor analysis of PCB congeners and PAHs.

Analytical Laboratory Group Analysis of Leachate and Sediment.Leachate and sediment were analyzed for concentrations

of selected PCB 1248 congeners, PAHs, and the heavy metalsidentified in Table V. Concentrations of PAH and PCBcongeners in leachate samples following methylene chlorideextraction were determined on either a Hewlett Packard 5985AAgas chromatograph/mass spectrophotometer equipped with aflame ionization detector (PAHs) or a Hewlett Packard 5880A

. gas chromatograph equipped with an electron capture detector(PCBs) (58,59).

Leachate and sediment samples were analyzed for arsenic,cadmium, chromium, lead, and zinc. Arsenic was analyzed bythe Atomic Absorbtion Gas Hydride Technique (EPA method 206.3(60)) using a Perkin-Elmer model 305 atomic absorptionspectrometer coupled to a Perkin-Elmer MHS-10 hydride gener-ator. Zinc in concentrations less than 50 parts per billion(ppb) also used the technique described for arsenic.

45

Qa .Bonded

Foam Liner

;

il. "‘?’/

n -\

—„m» )

Figure 2. EPRI/Acurex rotary extractor used to tumble serial batch leachtest: samples for PAH"s and PCB congeners (47).

46

Cadmium, chromium, lead, and zinc concentrations greater than4

50 ppb were analyzed using a Spectrospan III DCP—Argon PlasmaEmmission Spectrometer unit (61). For cadmium, chromium, andlead concentrations less than 50 ppb, the Atomic Absorption,Furnace Technique was used (EPA methods: '213.2, 218.2, and239.2 (60)). Analysis equipment for the furnace techniquewas a Perkin-Elmer model 500 hot graphite atomizer coupledto a Perkin—Elmer model 5000 atomic adsorption spectrometer.

Total organic carbon in the leachate and sediment was_ determined using the Combustion method (EPA method 415.1

(60)). The combustion method converts organic carbon to CO2,which is then measured by a flame ionization detector. AnOceangraph International Corporation total carbon system an-alyzer was used for this analysis.

DETERMINATION OF CONTAMINANT CONCENTRATION IN LEACHATE ANDSEDIMENT

This section describes how the concentrations of con-taminant in both the sediment and leachate were determined.Theory was developed and is currently being refined by Myerset al (62). The following discussion was extracted fromtheir work.

Chemical leach data were reduced to solid and aqueousphase concentrations using the calculations described below.

Solid phase contaminant concentration after leaching is givenby

47

Solidified Solidified Mass ofSediment Sediment ContaminantContaminant Contaminant LeachedConcentration = Concentration - ------—---After Before Mass SolidifiedLeaching Leaching Sediment Leached

or

q = qu — C (V/M) (3-1)

where: _q = total contaminant concentration in the solid phase

after leaching, mg/kg,q„ = initial contaminant concentration in the solidphase, mq/kq,C = contaminant concentration in the leachate, mg/l,

V = volume of aqueous phase (leachate), l, andM = mass of solidified sediment leached, kg.

Equation (3-l) relates to aa single contaminant. Since theliquid-solids ratio is given by

L/S = V / M (3-2)

where: k

L/S = liquid to solids ratio, ml/g,

V = volume, l, and

M = mass, kg.

Equation 3-l can be written as

48 (

q = qa - C (L/S) (3-3)

Equation 3-1 was used to calculate the solid phase concen-tration, q, corresponding to the aqueous phase concentration

determined by chemical analysis for the liquid-solids ratio(L/S) used. Metals, arsenic, and TOC tests used 100 ml ofdistilled-deionized water, the liquid-solids ratio is 100 mldivided by the mass of solidified/stabilized sediment leachedin grams. For the PAH and PCB congeners, the liquid-solidsratio is 1000 ml divided by the mass of solidified/stabilizedsediment leached in grams. '

Initial solid phase concentration for each contaminantis given by the relationship: ·

S‘*„ ’ nvüwi """)where

4

SX = contaminant concentration in the sediment before' solidification, mg/kg (dry weight basis),

w = moisture content of the wet sediment,kg water/kg sediment solids, and

R = dosage of solidification/stabilization reagents,kg reagents/kg wet sediment processed

The moisture content was 88 per cent, and values for SX are·

given in Table VIII. ·

49

TABLE VIII. CONTAMINANT CONCENTRATION IN THE SEDIMENTBEFORE SOLIDIFICATION (SX)

Contaminant SX, mg/kg (dry wgt)

MetalsArsenic 29.5Cadmium 20.0Chromium 282.0Lead 879.0Zinc ‘ 4125.0

Total Organic Carbon 24000.0

Polyaromatic HydrocarbonsAcenaphthene 96Acenapthylene 22Anthracene 62Benzo(a)anthracene 86Benzo(b)fluoranthene 140Benzo(a)pyrene 87Benzo(G H I)pery1ene 35Chrysene 92Fluoranthene 150Fluorene 69Indeno(1,2,3-C D)pyrene 50Naphthalene 2000Phenathrene 200Pyrene 140

Polychlorinated Biphenyl Congeners24(2-CL) Biphenyl 0.00224\(2-CL) Biphenyl 10.800244\(3—CL) Biphenyl . 19.50023\4\5(4—CL) Biphenyl 31.90022\45\(4-CL) Biphenyl 3.50022\55\(4¥CL) Biphenyl 19.50022\46(4-CL) Biphenyl 19.30022\3\45(5—CL) Biphenyl 5.24022\455\(5-CL) Biphenyl 1.66022\3a5\(5—cL) Biphenyl 5.70022\344\5\(6-CL) Biphenyl 3.61022\44\55\(6—CL) Biphenyl 2.28022\33\66\(6—CL) Biphenyl 0.00222\3456\(6—CL) Biphenyl 2.40022\334\55\(7—CL) Biphenyl 2.090

CHAPTER 4. RESULTS AND DISCUSSION

Determination of successful application <1f this~

solidification/stabilization technology was made kqr evalu-ation of physical and chemical stabilization, specifically,unconfined compressive strength and the serial batch leach

test. Solidification reagents added to the dredged material

changed the original sediment from a condition where it was

at or below its liquid limit to a material with a consistencyranging from a loamy soil to concrete-like state. Chemicalleachability'was measured for arsenic, cadmium, chromium,

lead, zinc, total organic carbon, polyaromatic hydrocarbons,and polychlorinated biphenyls.‘ The formulations were evalu-ated for effectiveness, separately for arsenic, metals, totalorganic carbon PAHs and PCBs and organics. ‘

RESULTS

Physical Stabilization

All process and. process formulations solidified the _

contaminated dredged material. Results of physical stabili-

zation research are depicted in Figures 3 through 8, which'

are plotted as strength (unconfined compressive strength) in

pounds per square inch (psi) versus cure time in days. Datapoints on the curves represent the mean unconfined

50

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compressive strength. Standard deviation for the data aver-

aged approximately 14.8 psi.

Cure times for all process formulations except Portlandcement are depicted for a ninety—day testing period, whilePortland cement is plotted through twenty—eight days. Figure3 shows a comparison of a high strength Portland cement for-mulation versus a FIRMEX with Portland cement formulation.Unconfined compressive strength for various formulations ofPortland cement, FIRMEX, and FIRMEX with Portland cement are

shown in Figures 4, 5, and 6, respectively.

Strength versus cure-time curves were also developed forPortland cement with West—Paine polymer, Figure 7, and FIRMEX

with West—Paine polymer, Figure 8, to complement the chemical °

leach studies conducted on Indiana Harbor sediment. Thepurpose of the polymer was to reduce leachability of organiccontaminants.

Chemical Stabilixation

Data produced from analysis of leachate from variousprocess formulations are presented in Tables A-I through

A-XXIV in the Appendix. The tables are organized by process

and formulations. Tables A-I through A-XVI present the re-sults of the arsenic, metals, and total organic carbon

leaching data. Results of PAH analysis are depicted in Ta-bles A-XVII through A-XX. PCB 1248 congener results are

58

shown zhi Tables A-XXI through A-XXIV. Each Table containsdata for one process formulation.

For Tables A-I through A-XVI, the first column providesmass in grams of dry, ground, solidified sediment leached per1OO milliliters distilled-deionized water. In the next col-umn, the liquid-solids ratio is expressed as milliliters pergram of solidified sediment. The remainder of the Table

provides the contaminant concentration in the leachate meas-ured in milligrams per liter and contaminant concentration

· in the solidified sediment after leaching measured in milli-

grams per kilogram.

Tables A-XVII through A-XXIV are arranged to accommodate

the large quantity of compounds analyzed. Organic contam-

inants are located in the first column of the Table. PAHsare listed alphabetically, however, PCB 1248 congeners arelisted in order from most water soluble to least water solu-ble. Numbers to the left of the contaminant are used to

provide a numerical listing to be referenced in later Fig-ures. The remainder of the Table provides the contaminantconcentration in the leachate measured in milligrams per li-ter and contaminant concentration in the solidified sediment

after leaching measured in milligrams per kilogrmn. These

columns are listed in descending order from the highest to

lowest liquid—solids ratio.

59

DISCUSSION

Physical Stabilization

All processes and formulations used were successful insolidifying Indiana Harbor sediment. The sediment requiredno preparation prior to addition of solidification reagents.Moisture present in the sediment was consumed by formationof hydration products, therefore dewatering was not required.

I Additional water was not required in the solidificationprocess. The original sediment was at or below its liquidlimit (average sample moisture content was measured at

eighty-eight percent). Solidified sediment exhibited

strengths that were above the range normally associated with

hard clay and solidified industrial sludge and below that

normally associated with soft concrete (see Table IV). Such

strengths are adequate to allow conventional landfill con-

struction equipment to operate on the solidified sediment.

Additionally, the handling characteristics of the solidified

sediments are significantly superior to those of the originalsediment.

The range of product strengths (56.7 to 721.6 psi) is

indicative of the versatility and flexibility of

solidification as a treatment process for immobilizing con-

taminated solids. Ten percent FIRMEX with twenty percent

Portland cement was determined to be the most effective for-

mulation for physical stabilization. It achieved a greater

60

unconfined compressive strength than thirty percent Portland

cement (see Figure 3). This is significant economically be-cause FIRMEX is somewhat less expensive than Portland cement

·(19).

Increased quantities of Portland cement produced a

higher unconfined compressive strength as expected (see Fig-

ure 4), whereas there was not a significant difference instrength for varying FIRMEX mix ratios (see Figure 5). When

FIRMEX and Portland cement are ‘used ixx combination, to

solidify sediment, there appears to be a synergistic effect(see Figure 6). Strengths achieved were certainly higher

than initially expected. As indicated in Figures 7 and EL

the unconfined compressive strength was increased by addition

of the polymer. A three percent addition of polymer.appeared

to be the optimum quantity to improve strength. Polymer

produced a sixty-four percent increase in strength for twenty

percent Portland cement. A seventy—two percent increase was

realized with fifty percent FIRMEX.

As indicated in Table V, the sediment contained grease,

oil, salts of zinc, copper, and lead which can interfere withE

the development of a hardened mass (24). The strength versus

cure—time curves, however, indicated that solidification did

occur. If the setting reactions responsible for

solidification were not occurring, the product would not gain

strength as they cured. This is a -significant result basedupon what is known about the potential for interference.

61l

Eormulations that included FIRMEX in the process did exhibita retarded set. whether this retarded set was caused bycontaminants in the sediment or is a function of FIRMEX isnot known.

It should be noted that cure time for all process for-mulations except Portland cement were measured through ninetydays. Pprtland cement was run only through twenty—eightdays. The first unconfined compressive strengths determinedwere for Portland cement. Initial testing intervals appearedreasonable as literature stated that cement reaches ninety-five percent of its final strength in twenty—eight days.FIRMEX formulations showed significant strength increases

beyond twenty—eight days. Accordingly, a decision was madethat testing would continue through ninety days.

Chemical StabilizationContaminant concentrations in the leachate were very

low. In fact, leachate concentrations were several ordersof magnitude less than that found 511 the sediment before

solidification. Total organic carbon showed the greatest

amount of leaching. Contaminant concentrations in the

leachate were only two to three orders of magnitude less thanthe untreated sediment concentration. Metals and PCBs proved

to be the most resistant to leaching as contaminant concen-trations in the leachate were four to five orders of magni-

tude lower than that found in the untreated sediment.

62

Resistance of arsenic and PAHs to leaching were less thanthat seen for metals and PCBs. Leachate concentrations of

arsenic and PAHs were three to four orders of magnitude lowerthan sediment concentrations.

l

Immobilization of contaminants varied between proc-

esses. No single process was found to be effective for all

contaminants. However, an individual single process may have

been more effective for a single contaminant or group of

contaminants. The following discussion provides an analysis‘ of process effectiveness for arsenic, metals, total organic

carbon, PAHs, and PCB 1248 congeners.

Arsenic and Metals. Analysis of the data for arsenic and the

metals revealed that in many cases contaminant concentration

in the leachate was below detection limit especially at the

highest liquid-solids ratios. Zinc and cadmium were the most

effectively immobilized contaminants in the solidified

sediment compared to arsenic and the other metals. Table IX

provides an analysis of leaching results. Solidified

sediment that showed no leachate contaminant concentrations

above the detection limit, at all liquid-solids ratios, were

said to release no contaminant. This is depicted in Table

IX as "N". Where contaminant concentration was below the

detection limit at all but the lowest liquid-solids ratio,the solidified sediment was said to have low contaminant re-

lease characteristics. This is depicted in the Table as "L".

63

TABLE IX. ANALYSIS OF ARSENIC AND METALS LEACHATE DATASHOWING SIGNIFICANT CONTAMINANT IMMOBILIZATION

Process Formulations(Percent by Weight of VReagent to Sediment) Arsenic Cadmium Chromium Lead Zinc

Portland Cement10 N * M L20 L * * M30 L N#40 L N

FIRMEX40 ‘

* * M* N50 N * * N60 . N * N

FIRMEX and Portland Cement20:10 M N * N10:20 L N * N15:15 L N * VN

Polymer and Portland Cement1:20 M L * N3:20 M N * N#*5:20 M N * * N#*

Polymer and FIRMEX _1:50 M * * M N3:50 ° M N * ND N5:50 M N * M N

N = No release of contaminant into aqueous phase at all liquid/solids ratios

L = No release of contaminant into aqueous phase except at thelowest liquid/solids ratio

M = Release of contaminants into aqueous phase except at the firstor second highest liquid/solids ratio

* = Greatest leachate contaminant concentration exhibited middleliquid/solids ratio

# = Had one or two aqueous phase concentration values abovedetection limit

ND = No data

64

Contaminant release in several solidified sediment samples

were characterized as moderate release where leachate con-

taminant concentrations were below the detection limit at the

first or second highest liquid—solids ratios. "M" is used

to indicate this occurrence in the Table.Analysis of the Table provides a clear assessment of

process effectiveness for zinc and cadmium and a basis for

assumptions concerning arsenic. Processes containing FIRMEX „

are the most effective for immobilizing zinc. Cadmium wasA

· effectively immobilized with a few exceptions by all proc-

esses evaluated. Arsenic seemed to be most effectively

immobilized by Portland cement; however, when the average

aqueous phase concentration of arsenic in the lowest liquid-

solids ratio were plotted as a histogram (see Figure 9), the

results conflicted with Table IX„ This Figure showed that

the most effective processes were the FIRMEX and Portland

cement formulations. FIRMEX used as the sole solidification

reagent was several times as ineffective as the other proc-

esses in immobilizing arsenic. It would appear that Portland

cement is contributing more to the immobilization of arsenic

than other solidifying additives. FIRMEX is the more effec-

tive solidification reagent for cadmium and zinc.

No release, low release, and moderate release charac-

terizations are useful in evaluating the data. Evaluation

of process effectiveness for immobilizing arsenic, cadmium

and zinc was done in this manner. Chromium and lead, how-

65

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66

ever, could not be characterized in this manner. Although

chromium, and wwith some exceptions lead, leached in all

process formulations and liquid-solids ratios, the quantity

of contaminant leached were four to five orders of magnitude

V lower than sediment concentrations. When there were suffi-cient data to analyze, process effectiveness could be deter-

mined by plotting desorption isotherms to determine

desorbable and nondesorbable quantities of contaminant. This

provides a more objective analysis of process effectiveness

than through comparison of a single liquid-solids ratio. The

data for chromium, however, showed no relationship between

aqueous phase concentration and sediment phase concentration

that would allow for interpretatmma as an isotherm. The

highest aqueous phase concentration of chromium occurred most

frequently at the mid—range liquid-solids ratios. To compare

process effectiveness, the highest aqueous phase concen-

trations in a series of liquid-solids ratios were averaged

and plotted as a histogram (see Figure 10). The high

Portland cement and polymer FIRMEX formulation proved to be

the most effective processes for contaminant immobilization.

The data for lead was also analyzed as a histogram be-

cause only half of the data could be plotted as an isotherm.

Figure 11 depicts the average aqueous phase concentration of

lead at the lowest liquid-solids ratio. As shown, the FIRMEX

additive resulted in the most effective immobilization of

lead, which the least effective was Portland cement. Addi-

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tion of polymer appeared to lessen the effectiveness of theFIRMEX.

_ The analysis of arsenic and metals can be summarizedinto several generalizations. Solidification is an effective

methodology for immobilization of those contaminants studiedi11 this ‘research. This .is especially true for cadmium.FIRMEX ‘was the most. effective solidification. reagent. for

immobilizing zinc and lead. Portland cement was more effec-

tive for arsenic and chromium.

Total Organic Carbon. Analysis of total organic carbon (TOC)data revealed that there was more leaching than that seen for

arsenic and the metals. Aqueous phase concentrations of TOCwere three orders of magnitude less than that found in the

sediment. All aqueous phase concentrations measured were

_ above the detection limit. ”

Data generated for TOC displayed a well-defined re-lationship between the aqueous phase concentration and thesolidified sediment phase. Pt was determined that becauseof this well-defined relationship that Langmuir isotherms(63) would be appropriate in evaluating process effective-

ness. An approximation of°a1 desorbable and nondesorbablefraction of TOC in the solidified sediment can be made byfitting· a Langmuir isotherm to the data. Normally* the

VLangmuir isotherm runs through the origin, however, this de-

scribes adsorption. To determine the difference between the

70i

desorbable and nondesorbable fractions, a plot of the

isotherm ix; passed through the ordinate in an approximate

location based upon fitting the curve to the data points.

This intercept is referred to as that amount of contaminant

resistant to leaching in the solidified sediment as depicted

in Figure l. The Langmuir isotherm equation is described

below (64):

(4-1)where:

q = contaminant concentration in the sediment phase

after leaching, mg/kg,

Q = saturation concentration in the sediment, mg/kg,

b = an empirical constant, and,

C = aqueous phase concentration, mg/l.

To determine if the Langmuir isotherm is appropriate to de-

scribe the data and to determine the saturation concentration

and empirical constant the data must be linearized using

equation 4-2 below (64). ·

A plot of C/q versus C approximates a line with a.slope 1/Q

and an intercept 1/bQ. If a linear plot cannot be drawn, then

the Langmuir isotherm is not applicable.

All the TOC data could be fitted to a Langmuir isotherm.

A typical isotherm is depicted in Figure 12. The results of

71

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analysis of the TOC data are summarized in Table X. Table Xis ordered from the most effective to least effective process

formulation. The higher strength polymer and FIRMEX formu-

lations proved to be the most effective solidification rea-

gents for immobilization of TOC contaminants. Comparison of

saturation concentrations derived from Equation 4-2 and the

contaminant concentration of the sediment phase at the lowestliquid-solids ratio in Tables A-I through A-XVI revealed that

TOC was at or near the saturation concentration in the

sediment.

Polyaromatic Hydrocarbons and Polychlorinated Biphenyls.

Analysis of polyaromatic hydrocarbon (PAH) and

polychlorinated biphenyl (PCB) 1248 congener data reveals

that for all processes evaluated the contaminant concen-

tration in the leachate was extremely small. For PAHs the

aqueous phase concentrations ranged from no contaminant in

. the leachate to a concentration that was four orders of mag-

nitude less than the sediment phase concentration. PCB 1248

congeners showed an even greater resistance to leaching with

more than half of the contaminants not releasing from the ‘

sediment. Where leaching, the contaminant concentration was

four to five orders of magnitude less than that found in the

sediment.

Classificatmma of data for PAHs and PCBs from serial

batch leaching tests conductad on solidified contaminated

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74

dredged material are presented in Tables XI and XII. When

Table XI is analyzed, polymer and FIRMEX appears to be the

most effective stabilization reagent because of the number

of no-release contaminants. The polymer and Portland cement

formulation. is nearly as effective. For the PAHs that

leached from the sediment, a histogram was prepared (see.

Figure 13). Evaluation of the histogram as a whole verifies

the initial determination of process effectiveness, however

FIRMEX is the most effective stabilization reagent for

naphthalene. Portland cement was the least effective sta-

bilization reagent with respect to PAHs.° Portland cement was determined to be the most effective

solidification reagent for the PCB 1248 congeners. The

polymer and FIRMEX formulations were nearly as effective as

the Portland cement. In all of PBC 1248 congener testing,

there were only two instances of a leachate contaminant con-

centration being greater than O.5 ppb, these being with the

more water soluble congeners. Figure 14 depicts a histogram

of the congeners that did leach. This histogram verifies the

analysis of Table XII, that Portland cement is the most ef-

fective process with the polymer and FIRMEX formulations be-

ing nearly as effective.

Figures 13 and 14 were generated using the highest

aqueous phase concentration for a series of liquid-solids

ratios. The lowest liquid-solids ratio did not always

75

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produce the highest value. This produced results that were

consistent with analysis of Tables XI and XII.

Frequently the data displayed a phenomenon of increasing

contaminant concentration in leachate in the three highest

liquid-solids ratios followed by a decrease in the two lowest

liquid-solids ratios. When the liquid-solids ratio versus

contaminant concentration is plotted, it approximates a

bell—shaped curve. An example of this phenomenon is depicted

for naphthalene in Figure 15. Di Toro et al. (65) describes

this as particle-particle interaction. Particle—particle

interaction does not occur at kdgher liquid-solids ratios

because sediment mass is small. Particles are surrounded by

a preponderance of leachant molecules and interaction is be-

tween particle and leachant molecules. When the liquid-solid

ratio is low and sediment mass is large, particle interaction

occurs between particles more than with leachant molecules.

As a result a smaller amount of contaminant is released.

Contaminant concentration in the leachant is also affected

by the fact that the organics evaluated have very low water

solubilities and more readily partition in sediment than wa—

ter. There were also many other contaminants present that

could interact with each other, such as grease and oil, and

effect partitioning. Another explanation is that the serial

batch leaching test may require a longer duration to allow-

the contaminant to reach equilibrium in the aqueous andsediment phases.

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Relationship Between Physical and Chemical Stabilization

A relationship between physical and chemical stabiliza-

tion was not established in this research. It was determined

that all processes and process formulations dewatered the

contaminated dredged material and produced a solidified mass.

Contaminant immobilization was substantial and in some in-

stances complete. The serial batch leach test represents the

worst case for leaching. Solidified sediment surfaces that

normally would be in contact with other sediment surfaces

are, as a result of grinding the solidified sediment, exposed

to a greater leachant concentration. Solidified sediment in

this case is not exhibiting one of its primary attributes,

that of presenting a solidified matrix resistant to intrusion

by leachant.

CHAPTER 5. CONCLUSIONS

Laboratory scale application. of' solidification/' sta-

bilization technologies to contaminated dredge material pro-

vided for the following conclusions to be drawn:

a. Physical stabilization of contaminated dredge nmterial

is a viable treatment option„ Application of cement-based

and. pozzolanic—based. processes uses the moisture in the

sediment to form hydration products, therefore, dewatering

is not required. All process formulations applied to the

contaminated dredged material produced a solidified sediment.

Twenty percent Portland cement with ten percent FIRMEX pro-

vided the highest unconfined compressive strength in

solidified sediment.

b. No single process formulation proved to be effective in

providing chemical stabilization for arsenic, metals, total

organic carbon, or organics. Solidification did provide a

significant amount of chemical stabilization. Aqueous phase

concentrations were lower than sediment phase concentrations

by as much as three to five orders of magnitude and in many

cases contaminants were completely immobilized.

1. Portland cement was the more effective solidifying

additive for arsenic, chromium, and PCB 1248 congeners. More

than half of the PCBs evaluated could not be detected in the

leachate of Portland cement solidified sediment. The PCBs

that did leach were measured at less than one ppb.

· 82

83

2. FIRMEX was more effective in immobilizing cadmium, _

zinc and lead. Zinc and cadmium were determined to be com-pletely immobilized because no detectable quantities werefound in the leachate.

3. West-Paine polymer was determined to be most effec-tive in reducing leaching of total organic carbon and PAHs.Total organic carbon concentrations in the aqueous phase werethree to four orders of magnitude less than the sediment

phase. Half of the PAHs were completely immobilized whilethe remaining PAH contaminants leached concentrations that

were four to five orders of magnitude lower than that found

in the original sediment samples.

LITERATURE'ClTED

1. Environmental Protection Agency, Corps of EngineersTechnical Committee on Criteria for Dredged and FillMaterials, 1977. "Ecological Evaluation of ProposedDischarge of Dredged Material into Ocean Waters." En-vironmental Effects Laboratory, US Army EngineerWaterways Experiment Station, Vicksburg, Mississippi39180-0631.

2, Reinisch, C. L., Charles, A. M., and Stone, A. M.,1984. "Epizootic neoplasia in soft shell clams col-lected from New Bedford Harbor," Hazardous Wastes, 1:1, p. 73.

3. Otouki, T., 1984. "The relationship between sedimentsand benthos in Mikawa Bay." Management of BottomSediments Containing Toxic Substances, EPA—600/3-78-084, US Environmental Protection Agency,. Corvallis, OR 97330.

4. Nishimura, H. and Kumagai, M., 1982. "Mercury pol-·lution of fishes in Minomata Bay and surrounding water:analysis of pathway of mercury," Soil, Air, and WaterPollution.

5. Young, D. R., McDermott, D. J., and Hessen, T. C.,1976. "DDT in sediments and organisms around southernCalifornia outfalls," JWPCF 48: 8, pp. 1919-1928.

6. Edgar, C. E. and Engler, R. M., 1984. "The LondonDumping Convention and Its Role in Regulating DredgedMaterial: An Update," Dredging and Dredged MaterialDisposal, American Society· of Civil Engineers, NewYork, p. 140-149.

7. Francingues, N. R., Jr., Palmero, M. R., Lee, C. R.,and Peddicord, R. K., 1985. Management Strategy forDisposal of Dredged Material: Contaminant Testing andControls. MP D-85-1, US Army Engineers Waterways Ex-periment Station, Vicksburg, MS 39180-0631.

8. Phillips, K. and Malek, J., 1984. "Dredging as a Re-medial Method for a Superfund Site," Dredging andDredged Material Disposal, American Society of CivilEngineers, New York, p. 634-643.9. Tittlebaum, M. E., Seals, R. K., Cartledge, F. K., and

”Engels, S., 1985. "State of the Art on Stabilization

C84

85

of Hazardous Organic Liquid Wastes and Sludges," Crit-ical Reviews in Environmental Control, 15: 2, p.179-211.

10. Malone, P. G., Jones, L. W., and Larson, P. J., 1980."Guide to the Disposal of Chemically Stabilized andSolidified Waste," SW-872, US Environmental ProtectionAgency, Cincinnati, Ohio.

11. Francingues, IL R., Jr., 1984. "Identification ofPromising Concepts for Treatment of ContaminatedSediments." 10th .Annual US-Japan Experts Meeting,Management of Bottom Sediments Containing Toxic Sub-stances, p. 139-165.

12. Lubowitz, H. R., Telles, R. W., Eliash, B. M., andUnger, S. L., 1984. "Contaminant Fixation: Practiceand Theory." Proceeding Tenth Annual Research Sympo-sium: Land, Disposal of Hazardous Waste, EPA-600/9-84-007, p. 205-210, US Environmental ProtectionAgency, Cincinnati, OH. .

13. Pozasek, P. B., 1979. Toxic and Hazardous Waste Dis-posal: Volume 1. Processes for· Stabi1ization/Solidification. Ann Arbor Science, Ann Arbor, MI.

14. Malone, P. G., and Larson, R. C., 1983. "ScientificBasis of Hazardous Waste Immobilization," Hazardous andIndustrial Solid Waste Testing, Second Symposium, STP805, American Society for Testing and Materials,Philadelphia, PA.

15. Malone, P. G., and Jones, L. W., 1979. "Survey ofSolidification/Stabilization Technology for Hazardous~ Industrial Wastes," EPA-600/2-79-056, US EnvironmentalProtection Agency, Cincinnati, OH.

16. Mahloch, J. L., Averett, D. E., and Bartos, M. J.,1976. Pollutant Potential of Raw and Chemically FixedHazardous Industrial Waste and Flue Gas DesulfurizationSludges. EPA—60/2-76-182, U.S. Environmental Pro-tection Agency, Cincinnati, OH. 117 pp.

17. Mahloch, J. In Leachability and Physical Propertiesof Chemically Stabilized Hazardous Wastes. Presentedat Environmental Protection Agency, Hazardous WasteResearch Symposium, Tucson, Ariz., February 2 ‘¤¤ 4,1976.

18. Burk, IH. R., Denham, R., and Lubowitz, H., 1974. Re-commended Methods of Reduction, Neutralization, Recov-

36

ery or Disposal of Hazardous Wastes. Vol. 1Y TRWSystems Group, Inc., Redondo Beach, Calif. 89 pp.19. Myers, T. E., 1985. Personal communication.20. Labovitz, C., and Hoffman, D. C., l979„ "Effective

disposal of fine coal refuse and flue gasdesulfurization slurries using calcilox additive sta-bilization technique," in Toxic and Hazardous WasteDisposal, Vol. 1, Pojasek, R. B., Ed., Ann Arbor Sci-ence, Ann Arbor, Mich., 93.

21. Krofchak, D., 1979. "Solidification of waste, in Toxicand Hazardous Waste Disposal," Vol. 1, Pojasek, R. B.,Ed., Ann Arbor Science, Ann Arbor, Mich., p. 349.

22. Musser, D., Nov. 1985. ENRECO. Personal communi-cation.

23. Christensen, ID. C., and Wakamiga, W., 1980. "A solid _future for solidifiction/fixation process," 511 Toxicand Hazardous Waste Disposal, Vol. 4, Pojasek, R. B.,Ed., Ann Arbor Science, Ann Arbor, Mich., p. 75.

24. McNeese, J. A., Dawson, G. W., and Christensen, D. C.,1979. "Laboratory studies of fixation of kepone-contaminated sediments," in Toxic and Hazardous WasteDisposal, Vol. 2, Pojasek, R. B., Ed., Ann Arbor Sci-ence, Ann Arbor, Mich., p. 217.

25. Jones, J. N., Bricka, R. M., Myers, T. E., Thompson,D. W., 1985. "Factors Affecting Stabilization/Solidificatiqn of Hazardous Waste," Proceedings:International Conference on New Frontiers for HazardousWaste Management, EPA/600/9-85/025, p. 320-327, US En-vironmental Protection Agency, Cincinnati, OH.

26. Meyers, T. E., Francingues, N. R., Jr., and Thompson,ID. W., 1985. "Sorbent Assisted Solidification of aHazardous Waste," Proceedings: International Confer-ence on New Frontiers for Hazardous Waste Management,EPA-600/9-85-025, p. 348.

27. Proposal to Chicago District, Corps of Engineers, forApplication of Innovative Techniques for Disposal ofHighly Contaminated Sediments: Phase 1, 10 Oct 1984,Environmental Labortory, Waterways Experiment Station,Vicksburg, MI 39180.

28. Ludwig, D. D., Sherrard, J. H., Betteker, J. M., 1985."Implementation Strategies for Application of

87

Solidifed/Stabilization Technology to Dredged Mate-rial," Virginia Polytechnic Institute and State Uni-versity, Final Report. Submitted to the ·U.S. ArmyCorps of Engineers Waterways Experiment Station, Con-tract DACW 39-85-M-5086.

29. Kita, D., and Kmbo, IL, 1983. "Several SolidifiedSediment Examples," 7th US/Japan Experts Meeting, Man-agement of Bottom Sediments Containing Toxic Sub-stances. Water Resource Support Center, Ft. Belvoir,VA., U.S. Army Corps of Engineers, p. 194.

· 30. Kamon, M., 1984. "Lime-Cement Hardening of Very SoftFresh Water Clay," 10th Annual US-Japan Experts Meet-ing, Management of Bottom Sediments Containing ToxicSubstances, p. 213-235.

31. Murakami, K., 1977. "An Experiment in Removal of Or-ganically Polluted Bottom Mud from the Seto InlandSea," Proceedings, Management of Bottom Sediments Con-taining Toxic Substances, EPA-600/3-73/083, p. 62.

32. Okumury T., 1976. "Chemical Stabilization of SoftSoils," Proceedings, Management of Bottom SedimentsContaining Toxic Substances, EPA-600/3-77-083, p. 155.

33. Oshita, N., 1981. "On the New Method of Treating Bot-~ tom Sediment by a Silicic Coagulant (SIL-B Treatment· Method)," Proceedings 6th Management of BottomSediments Containing Toxic Substances, p. 256.

34. Otsuki, T., and Shima, M., 1982. "Soil Improvement byDeep Cement Continuous Mixing Method and Its Effect onthe Environment," Japan Dredging and Reclamation Engi-neering Association, p. 215.

35. Tabuse, I., 1981. "How to Dredge-up and Treat BottomSediment in the River Waka," Proceedings 6th Managementof Bottom Sediments Containing Toxic Substances, p.239.

36. Krizek, R. J., et al., 1977. "Chemical Stabilizationof Dredged Materials," Proceedings, ASCE Conference onGeotechnical Practice of Solid Waste Disposal, U. ofMichigan, p. 517. _

37. Bartos, M. J., and Palermo, M. R., 1977. Physical andEngineering Properties of Hazardous Industrial Wastesand Sludes. EPA-600/2-77-139, US Environmental Pro-tection Agency, Cincinnati, OH.

88

38. Bricka, R. M., 1985. Personal communication.

39. Hannak, P. K., 1985. Correspondence with T. E. Myers,dated 15 Oct 1985.

40. Terzaghi, K., Peck, R. B., 1967. Soil Mechanics inEngineering Practice. John Wiley and Sons, Inc., NewYork, NY.

41. Lowenbach, William, 1978. Compilation and Evaluationof Leaching Test Methods. EPA-660/2-78-095, USEPA,Cincinnati, OH 45268.

42. Hespe, I. C. D., 1971. "Leach Testing of ImmobilizedRadioactive Waste Solids," Atomic Energy Review, 9: p.195.

43. Conway, R. A., and Malloy, B. C., 1981. HazardousSolid Waste Testing: First Conference, STP 760, Amer-ican Society for Testing and Materials, Philadelphia,PA.

44. Conway, R. A., and Gulledge, W. P., ed., 1983. Haz-ardous and Industrial Solid Waste Testing, 2nd Sympo-sium. ASTM STP 805, Am. Soc. for Testing andMaterials, Philadelphia, PA.

45. Jackson, L. P., Rohlik, A. R., and Conway, R. A., 1984.Hazardous and Industrial Waste Management and Testing,3rd Symposium. ASTM STP 851, American Society forTesting and Materials, Philadelphia, PA.

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