ENVIRONMENTAL RESTORATION of METALSCONTAMINATED SOILS - CHAPTER 1 pdf

During recent decades, phenomenal progress has been made in several areas of biology,ecology, health, and environmental geochemistry of heavy metals in soils.. The cleanup techniques mos

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ENVIRONMENTAL RESTORATION of

CONTAMINATED

METALS-SOILS

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Edited by

I.K Iskandar

ENVIRONMENTAL RESTORATION of

CONTAMINATED

METALS-SOILS

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Environmental restoration of metals-contaminated soils / edited by I.K Iskandar.

p cm.

Includes bibliographical references and index.

ISBN 1-56670-457-X (alk paper)

1 Metals—Environmental aspects 2 Soil remediation I Iskandar, I K (Iskandar Karam), 1938–

TD879.M47 E58 2001

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During recent decades, phenomenal progress has been made in several areas of biology,ecology, health, and environmental geochemistry of heavy metals in soils Prior to the1960s, research was focused on enhancing the plant uptake or availability of selected heavymetals or minor elements (also referred to as micronutrients) from the soil More recently,concerns regarding heavy metals contamination in the environment affecting all ecosystemcomponents, including aquatic and terrestrial systems, have been identified with increas-ing efforts on limiting their bioavailability in the vadose zone

Recently, many sites have been identified as hazardous waste sites because of the ence of elevated concentrations of heavy metals In some cases, contamination of ground-water with metals that have potential health effects has also been discovered The totalmass of metals in surface soils is an important factor influencing their migration in the soil

pres-to the groundwater However, soil environmental conditions and physical, chemical, andbiological processes are also important factors affecting the fate of metals in soils

Unlike organic contaminants that can be destroyed (or mineralized) through treatmenttechnologies, such as bioremediation or incineration, metal contaminants cannot Once ametal has contaminated soil, it will remain a threat to the environment until it is removed

or immobilized The cleanup techniques most used for the remediation of heavy metalscontamination are excavation and subsequent landfilling of the heavy metals-contami-nated soil or waste (commonly referred to as “dig and haul”) Dig and haul does notremove the contaminant from the waste but simply transfers the contamination from onearea to another Usually, no effort is made to reduce the mobility of the heavy metalsbeyond containment in a secured landfill

Because of the concerns regarding the role of heavy metals in the environment, a series

of international conferences was held to explore the emerging issues of the try of trace elements in the environment In June 1997, the Fourth International Conference

biogeochemis-on the Biogeochemistry of Trace Elements was held in Berkeley, CA The cbiogeochemis-ontributibiogeochemis-ons inthis book were presented in part at this conference This book, Environmental Restoration of Metals-Contaminated Soils, follows earlier titles: Engineering Aspects of Metal-Waste Manage- ment, 1992, and Remediation of Soils Contaminated with Metals, 1997

The contributors are a multidisciplinary group of scientists and engineers; the bookwas written to update current information on environmentally accepted methods for siterestoration

The book is organized in 14 chapters The first eight chapters deal with the physical andchemical methods and processes for soil remediation The other six chapters focus onselected biological methods and processes for remediation

amendments for stabilization

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environmental restoration of selenium-contaminated soils Chapter 11 discusses trace ments in soil-plant systems under tropical environment The process of metal removal bychelation using amino acids is presented in Chapter 12 Chapter 13 examines the effects ofnatural zeolite and bentonite on the phytoavailability of heavy metals Chapter 14 discussesmetal uptake by agricultural crops from sewage sludge-treated soils.

ele-I thank the authors for their contributions ele-I am also grateful for their patience, valuabletime, and effort in preparing and critiquing the various chapters and in keeping the focus

on the main theme of soil remediation I gratefully acknowledge the technical reviews vided by Dr A.L Page of the University of California, Riverside

pro-Without the support of the Center for Environmental Engineering, Science and ogy (CEEST) at the University of Massachusetts, Lowell, and the U.S Army Cold RegionsResearch and Engineering Laboratory (CRREL), this project could not have been achieved

Technol-I thank Edmund A Wright (since deceased) and Donna Harp of CRREL for their editingand typing support Finally, I thank my wife, Bonnie Iskandar, for her encouragement andsupport and for allowing me to work at home many hours to complete this volume.This volume is dedicated to the memory of the late Edmund A Wright, who over the past

25 years provided me with technical editing

Iskandar K Iskandar

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Iskandar K Iskandar earned his Ph.D degree in soil science and water chemistry at theUniversity of Wisconsin–Madison, in 1972 He is a research physical scientist at the ColdRegions Research and Engineering Laboratory (CRREL) and a Distinguished Research Pro-fessor at the University of Massachusetts, Lowell He developed a major research program

on land treatment of municipal wastewater and coordinated a number of research areasincluding transformation and transport of nitrogen, phosphorus, and heavy metals Healso developed the Cold Regions Environmental Quality Program at CRREL which hemanaged from 1985 to 1997 His recent research efforts have focused on the fate and trans-formation of toxic chemicals, development of non-destructive methods for site assess-ments, and evaluation of in situ and on-site remediation alternatives Dr Iskandar hasedited several books and published numerous technical papers He organized severalnational and international workshops, conferences, and symposia He received a number

of awards including the Army Science Conference Award, CRREL Research and ment Award, and CRREL Technology Transfer Award Dr Iskandar is a fellow of both theSoil Science Society of America and the American Society of Agronomy, and vice president

Develop-of the International Society Develop-of Trace Element Biogeochemistry

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Sultana Ahmed Bangladesh Institute of Nuclear Agriculture, Bangladesh

Akram N Alshawabkeh Northeastern University, Department of Civil and EnvironmentalEngineering, Boston, Massachusetts 02115, U.S.A

Herbert E Allen Department of Civil and Environmental Engineering, University ofDelaware, Newark, Delaware 19716, U.S.A

Alain Bermond Institut National Agronomique Laboratoire de Chimie Analytique, Paris,France

R Mark Bricka U.S Army Corps of Engineers Engineering Research & DevelopmentCenter, Vicksburg, Mississippi 39180, U.S.A

Lenom J Cajuste Colegio de Postgraduados, Chapingo Montecillo, Mexico

Zueng-Sang Chen Graduate Institute of Agricultural Chemistry, National Taiwan versity, Taipei, Taiwan

Uni-K.S Dhillon Department of Soils, Punjab Agricultural University, Ludhiana, India

S.K Dhillon Department of Soils, Punjab Agricultural University, Ludhiana, India

James A Holcombe Department of Chemistry and Biochemistry, University of Texas,Austin, Texas 78712, U.S.A

Maury Howard Department of Chemistry and Biochemistry, University of Texas, Austin,Texas 78712, U.S.A

Achim Kayser Swiss Federal Institute of Technology, Institute of Terrestrial Ecology, SoilProtection Group, Zürich, Switzerland

Armin Keller Swiss Federal Institute of Technology, Institute of Terrestrial Ecology, SoilProtection Group, Zürich, Switzerland

Catherine Keller Swiss Federal Institute of Technology, Institute of Terrestrial Ecology,Soil Protection Group, Zürich, Switzerland

A.S Knox (formerly A Chlopecka) Savannah River Ecology Laboratory, University ofGeorgia, Aiken, South Carolina 29802, U.S.A

Reggie J Laird Colegio de Postgraduados, Chapingo Montecillo, Mexico

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Valérie Laperche Centre National de Recherche sur les Sites et Sols Pollués, Douai,France

Geng-Jauh Lee Graduate Institute of Agricultural Chemistry, National Taiwan University,Taipei, Taiwan

Suen-Zone Lee Department of Environmental Engineering and Health, Chia Nan College

of Pharmacy and Science, Tainan, Taiwan

Jen-Chyi Liu Department of Agricultural Chemistry, Taiwan Agricultural Research Institute,Council of Agriculture, Taichung, Taiwan

M.J Mench Centre Bordeaux-Aquitaine, INRA Agronomy Unit, Villenave d’Ornon,France

S.M Rahman Bangladesh Institute of Nuclear Agriculture, Mymensingh, Bangladesh

Rainer Schulin Swiss Federal Institute of Technology, Institute of Terrestrial Ecology, SoilProtection Group, Zürich, Switzerland

J.C Seaman Savannah River Ecology Laboratory Advanced Analytical Center for mental Science, University of Georgia, Aiken, South Carolina 29802, U.S.A

Environ-László Simon College of Agriculture, Gödöllõ University of Agricultural Sciences,Nyiregyhaza, Hungary

C.D Tsadilas Institute of Soil Classification and Mapping, National Agricultural ResearchFoundation, Larissa, Greece

J Vangronsveld Limburgs Universitair Centrum, Environmental Biology UniversitaireCampus, Diepenbeek, Belgium

Clint W Williford, Jr. Department of Chemical Engineering, University of Mississippi,Oxford, Mississippi

Yujun Yin Department of Civil and Environmental Engineering, University of Delaware,Newark, Delaware 19716, U.S.A

Sun-Jae You Department of Marine Environmental Engineering, Kunsan National sity, Republic of Korea

Univer-Isabelle Yousfi (deceased) IPSN\DPRE\SERGD\Laboratoire d’Étude des Stockages deSurface, Fontenay-aux-Roses, France

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Section I Physical and Chemical Methods and Processes

1 Physical-chemical approach to assess the effectiveness of

trace metals-contaminated soils by adding solid phases 3

Isabelle Yousfi and Alain Bermond

stabilization techniques 21

A.S Knox*, J.C Seaman, M.J Mench, and J Vangronsveld

Valérie Laperche

4 Determinants of metal retention to and release from soils 77

Yujun Yin, Suen-Zone Lee, Sun-Jae You, and Herbert E Allen

5 Chemical remediation techniques for the soils contaminated with

cadmium and lead in Taiwan 93

Zuen-Sang Chen, Geng-Jauh Lee, and Jen-Chyi Liu

6 Soil pH effect on the distribution of heavy metals among soil fractions 107

C.D Tsadilas

7 Physical separation of metal-contaminated soils 121

Clint W Williford, Jr and R Mark Bricka

8 Heavy metals extraction by electric fields 167

Akram N Alshawabkeh and R Mark Bricka

Section II Biological Methods and Processes

9 The relationships between the phytoavailability and the extractability ofheavy metals in contaminated soils 189

Lenom J Cajuste and Reggie J Laird

10 Restoration of selenium-contaminated soils 199

K.S Dhillon and S.K Dhillon

Sultana Ahmed and S.M Rahman

* Formerly A Chlopecka

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12 Polyamino acid chelation for metal remediation 243

Maury Howard and James A Holcombe

13 Effects of natural zeolite and bentonite on the phytoavailability of

heavy metals in chicory 261

László Simon

14 Heavy-metal uptake by agricultural crops from sewage-sludge

treated soils of the Upper Swiss Rhine Valley and the effect of time 273

Catherine Keller, Achim Kayser, Armin Keller, and Rainer Schulin

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Physical-Chemical Approach to Assess the Effectiveness of Several Amendments Used for In Situ

Remediation of Trace Metals-Contaminated Soils by Adding Solid Phases

Isabelle Yousfi (deceased) and Alain Bermond (corresponding author)

CONTENTS

1.1 Introduction 3

1.1.1 Remediation Techniques 4

1.1.2 In Situ Remediation by Adding Solid Phase 4

1.2 Example of Study to Assess the Effectiveness of Several Amendments 7

1.2.1 Methods 7

1.2.1.1 Soil Characteristics 7

1.2.1.2 Rapid Characterization of the Solid Phases Used as Amendments 8

1.2.1.3 Calculation of the Amendment Effect 10

1.2.1.4 Analytical Methods 13

1.3 Results and Discussion 14

1.4 Conclusion 17

References 20

The increasing use of trace metal-contaminated sewage sludge as agricultural fertilizer or the storage of polluted wastes can cause toxic elements to accumulate in soils After com-plex processes, these elements may pass into the soil solution where plant uptake or leach-ing to groundwater can contaminate the food chain

Thus, increasing contamination of agricultural soil by toxic compounds such as heavy metals, metalloids, or organic pollutants has important health and economic implications With this in mind, several cleanup methods have been investigated, which can be divided into two groups: those that remove contaminants, and those that transform pollutants into

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4 Environmental Restoration of Metals–Contaminated Soils

1.1.1 Remediation Techniques

Biological treatments generally consist of in situ remediation and biodegradation, relying

on microbiological activities to remove contaminants, which in most cases are organic lutants This technique is being used to remove HAPs or PBCs (Hamby, 1996) or to trans-form pollutants to harmless forms It is an immobilization technique involving, forexample, photolysis of organic compounds Another biological cleanup approach is thecultivation of plants, called hyperaccumulators, that are able to accumulate one or severaltoxic elements This method has been successfully used for different toxic trace elements,for instance Cd and Zn (Keller et al., 1997) or nickel (Homer et al., 1991)

pol-Physical treatments remove contaminants through physical means Among theseapproaches are thermal desorption or vapor stripping of semi-volatile or volatile com-pounds Electrokinetic migration, useful for anionic and cationic compound extraction, canalso be mentioned (Chapter 8)

Chemical treatments include all techniques involving reagents or external compounds.Soil washing is one In this technique different reagents able to solubilize toxic elements arecoupled with the removal of leaching solutions and added chelators that make cations lesslabile, thus allowing them to immobilize toxic elements in a less bioavailable form Forinstance, EDTA is one of the proposed complexing reagents (Li and Shuman, 1996) In addi-tion, adding solid phases should also be mentioned Solid phases can fix (irreversibly) toxicelements, and they can sometimes be used to reduce remediation costs

Among these different remediation techniques, this chapter focuses on this last method.Adding solid phases is an interesting and low-cost technique

1.1.2 In Situ Remediation by Adding Solid Phase

The question here is what will the effect be of adding the following different kinds of ments to contaminated soils: clay minerals, hydrous iron oxides (HFO), hydrous manganeseoxides (HMO), fly ashes, etc Two kinds of studies have been carried out The first type con-sists of plant studies, in which some authors conducted experiments on the effect of amend-ments on the uptake of trace elements by plants They did this by comparing the amounts

amend-of cadmium, lead, copper, or zinc in plants grown on contaminated soils with or withoutamendments (Gworek, 1992a, 1992b; Wong and Wong, 1990; Petruzzelli et al., 1987; Chlo-pecka and Adriano, 1997) For instance, Gworek (1992a) studied the effect of adding syn-thetic zeolites on the amount of Cd in lettuce, oats, and ryegrass She noted a significantdecrease in Cd in plant tissue in 85% of lettuce leaves and about 45% of lettuce roots.Chlopecka and Adriano (1997) worked with four different soils and studied the effect oftwo kinds of zeolite and apatite on the amount of Cd, Zn, and Pb in maize tissue Among theresults shown, they found a decrease of about 50% of Pb in maize leaves grown on a zeolite-amended soil, and a 20% reduction in Cd content in maize grown on apatite-amended soil.Fly ashes are used as agricultural amendments, too, particularly because they are low-cost wastes Petruzzelli et al (1987) have added from 0 to 5% (w/w) fly ash to soils andstudied the amount of Cu, Ni, Cr, and Zn in wheat seedlings Amendments seem to have auseful effect and result, for instance, in a decrease of about 65% of Zn in roots when 5% flyash is added Wong and Wong (1990) have also studied fly ashes and mixed coal fly ashes

at rates of 0, 3, 6, and 12% in two soils If they divided the amount of Zn in vegetables(cabbages) by a factor of two, the authors then noticed an increase of soil pH and a decrease

in several cases of the vegetal yield They concluded that there was a possible phytotoxiceffect of fly ashes However, the liming effect involved adding fly ashes, implying that thelowered bioavailability of oligo-elements can be another assumption, as Waren et al (1993)and Davies et al (1993) have assumed

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Physical-Chemical Approach to Assess the Effectiveness of Several Amendments 5

Although the range of effects varied with the plants studied, in most cases the ments brought about a reduction of trace metal concentrations in plant tissues However,

amend-in the case of fly ashes, an important variation of soil pH after application was noticed, and

a correlation between trace element concentrations in the plant and the pH of the amendedsoil was found (Wong and Wong, 1990)

In another approach to remediation, some authors studied the correlation between traceelements in plants and soils In this case, the quantities of trace metals in soils were deter-mined using chemical fractionation procedures, before and after the amendments A fewexamples can be given Pierynski and Schwab (1993) have studied the effect of limestone,

N Viro Soil, or phosphates on the content of Zn, Cd, and Pb in soybean tissues In othertests, chemical extraction procedures have been carried out on soils amended or not Bymeans of these protocols, they observed a redistribution of trace elements between soil frac-tions; in addition, several phases seem to improve plant quality Thus, they noted that lime-stone can decrease about 65% of Zn and 33% of Cd in plant tissue Adding N Viro Soilresulted in a decrease of 33% of Pb in leaves

Sappin-Didier et al (1994), after adding 1% (w/w) of steel shot to two different soil ples, have studied the amount of Ni, Cr, and Pb in ryegrass and tobacco Among theirresults, they showed that Cd can be decreased by 40% in tobacco Simultaneously, the frac-tions of extractable Cd H2O and Ca(NO3)2 decrease about 75 and 85%, respectively Withthe same plants, Mench et al (1994) have studied the effect of lime, HFO, HMO, andzeolites on different types of soils Among their results, they found that the amount of Cddecreases by 75% in ryegrass roots grown on HMO-amended soils and by 50% in tobaccogrown under the same conditions In addition, lead content in plant tissue significantlydecreases with HMO (–75%) or lime (–65%)

sam-Davies et al (1993) studied the effect of adding agricultural limestone to soils nated with different ranges of trace metals The EDTA extractable fractions of Cd, Pb, and

contami-Zn were studied before and after amendment; in addition, the total content of trace ments in radishes was investigated For single application, Davies et al (1993) noticed,under the best conditions, a decrease of Zn and Pb in vegetative tissue of about 20%, whilethe EDTA-extractable fraction of zinc and lead in soil also decreased

ele-From a general point of view, chemical extractions showed that the amendments resulted

in changes in the fractionation of trace elements available to crops

Amendments with solid phases such as fly ashes (Wong and Wong, 1990; Petruzzelli et al.,1987; Pierzynski and Schwab, 1993), limestone, K2PO4, or hydrous manganese oxides andhydrous iron oxides (Wong and Wong, 1990; Petruzzelli et al., 1987; Pierzynski and Schwab,1993; Sims and Kline, 1991; Mench et al., 1994) and zeolites (Gworek, 1992a, 1992b; Chlo-pecka and Adriano, 1997) can influence plant uptake, but unfortunately, these amendmentscan also influence the physicochemical parameters of the soil, particularly its pH Thesechanges influence the effectiveness of amendments, but they are rarely taken into account.Several studies mention the effect on pH value of adding solid phases For instance,Wong and Wong (1990) show that the pH value can increase from 1.5 to 2 units by addingalkaline fly ashes With fly ashes, too, Petruzzelli et al (1987) observed a decrease by a third

of Ni in roots, and they also observed simultaneous pH increases from 6.1 to 8.5 Davies et

al (1993) underline the accepted liming effect of agricultural limestone and note an increase

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