Heavy metal adsorption on iron oxide and iron oxide-coated silica ...

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LIST OF FIGURES(Continued)FigurePage10.3 Comparison of Ni <strong>adsorption</strong> isotherms on 5 g L -1 silica and goethite-coatedsilica (GACS, 4.01 mg Fe g -1 solid) and 1 g L-1 goethite at ionic strength (IS)10-3 as a function of pH. 14910.4 Ni <strong>adsorption</strong> isotherms on 5 g L -1 silica and goethite-coated silica (GACS,4.01 mg Fe g-1 solid) and 1 g L -1 goethite at ionic strength (IS) 10-3 as afunction of pH. 15010.5 Comparison of Zn <strong>adsorption</strong> isotherms on 5 g L-1 silica and goethite-coatedsilica (GACS, 4.01 mg Fe g -1 solid) at ionic strength (IS) 10-3 as a functionof pH 15310.6 Zn <strong>adsorption</strong> isotherms on 5 g L -1 silica and goethite-coated silica (GACS,4.01 mg Fe g -1 solid) and 1 g L -1 goethite at ionic strength (IS) 10-3 as afunction of pH. 154A.1 Ni solubility in open system at 298 K (in 10 -3 M NaNO3, PCO2=1 0-3.46 atm) 159A.2 Ni speciation in 1x10 -5 M Ni(NO3)2 in open system at 298 K (ionic strength10-3 NaNO3, PCO2=1 0-3.46 atm) 160A.3 Pb solubility in open system at 298 K (ionic strength 10 -3 NaNO3, PCO2=10 -3.46 atm). 161A.4 Pb speciation in 5x10 -8 M Pb(NO3)2 in open system at 298 K (ionic strength10-3 NaNO3, PCO2=1 0-3.46 atm) 162A.5 Zn solubility in open system at 298 K (ionic strength 10 -3 NaNO3, PCO2=10 -3.46 atm). 163A.6 Zn speciation in lx10-5 M Zn(NO3)2 in open system at 298 K (ionic strength10-3 NaNO3, PCO2=1 0-3.46 atm) 164xviii
CHAPTER 1INTRODUCTION<strong>Heavy</strong> <strong>metal</strong>s in natural aquatic and soil environments potentially impact the growth ofplants and threaten the health of animals and humans even when present in traceamounts. Risk assessment and remediation require information on heavy <strong>metal</strong>speciation, mobility, and bioavailability to characterize their behavior and impact in theenvironment. Sorption is one of the most important processes that influences thedistribution and transport of heavy <strong>metal</strong>s in aquatic and/or soil environments (Benjaminand Leckie, 1981a; Siegel et al. 1992).<strong>Heavy</strong> <strong>metal</strong> <strong>adsorption</strong> to hydrous iron, manganese, and aluminum oxides hasbeen extensively investigated (e.g., Forbes et al. 1976; Swallow et al. 1980; Hsi andLangmuir, 1985; Hayes and Leckie, 1986; Johnson, 1990; Cowan et al. 1991; Müller andSigg, 1992; Ainsworth et al. 1994; Manceau and Charlet, 1994; Coughlin and Stone,1995; Fendorf et al. 1997; Green-Pedersen et al. 1997; Venema et al. 1998; Jenne, 1998;Villalobos et al. 2001; Peak and Sparks, 2002; Dyer et al. 2003; Wazne et al. 2003;O'Reilly and Hochella, 2003; Kanungo et al. 2004; Jeon et al. 2004). These minerals areprevalent in natural environments as particles or surface coatings, have high affinity andgreat capacity for <strong>metal</strong> ions (Schwertmann and Cornell, 1991), and therefore impact<strong>metal</strong> contaminant mobility (e.g., Anderson and Christensen, 1988; Jackson and Inch,1989; Johnson, 1990; Coston et al. 1995; Fuller et al. 1996; Green-Pedersen et al. 1997;Dong et al. 2002). Although individual sorbents and contaminants have beeninvestigated, the presence of competing ions is more frequently encountered (e.g.,1
Page 1 and 2: Copyright Warning & RestrictionsThe
Page 3 and 4: ABSTRACTHEAVY METAL ADSORPTION ON I
Page 5 and 6: HEAVY METAL ADSORPTION ON IRON OXID
Page 7 and 8: APPROVAL PAGEHEAVY METAL ADSORPTION
Page 9 and 10: Fan, M.; Boonfueng, T.; Xu, Y.; Axe
Page 11 and 12: ACKNOWLEDGMENTI would like to expre
Page 13 and 14: TABLE OF CONTENTS(Continued)Chapter
Page 15 and 16: TABLE OF CONTENTS(Continued)Chapter
Page 17 and 18: LIST OF TABLES(Continued)TablePageB
Page 19 and 20: LIST OF FIGURES(Continued)FigurePag
Page 21: LIST OF FIGURES(Continued)FigurePag
Page 25 and 26: 3and Sigg, 1992; Gunneriusson et al
Page 27 and 28: CHAPTER 2OXIDES AND THEIR EFFECT ON
Page 29 and 30: 7et al. 1996; Green-Pedersen et al.
Page 31 and 32: 9identify components, distribution,
Page 33 and 34: 11oxides. Because extraction method
Page 35 and 36: 13Table 2.2 Some Coating Work and C
Page 37 and 38: 15increasing the sorbate concentrat
Page 39 and 40: 17mole Cu g-1 goethite (-1-7% of th
Page 41 and 42: 19Overall, macroscopic adso
Page 43 and 44: 21hematite (up to 9.9 limo' Pb ril-
Page 45 and 46: 23concentration in their system was
Page 47 and 48: 25Surface complexation modeling (SC
Page 49 and 50: 27Overall, surface complexation mod
Page 51 and 52: 29Spectroscopic techniques, especia
Page 53 and 54: 31• Understand the effect of comp
Page 55 and 56: 33existing in almost all soils and
Page 57 and 58: CHAPTER 4EXPERIMENTAL METHODSIn thi
Page 59 and 60: 37included coating temperature (T),
Page 61 and 62: 39generated at 45 kV and 40 mA, sca
Page 63 and 64: 41PZC include electrophoretic mobil
Page 65 and 66: 43Lin-edge, from 8,133 to 8,884 eV
Page 67 and 68: CHAPTER 5CHARACTERIZATION OF IRON O
Page 69 and 70: 47measured by potentiometric titrat
Page 71 and 72: Table 5.2 XRD Data of Alfa Aesar (A
Page 73 and 74:
51Table 5.3 XRF Results for Alfa Ae
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Figure 5.4 Particle size distributi
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55Figure 5.5 ESEM micrograph for Al
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585.2.5 Surface Charge Distribution
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Figure 5.10 Potentiometric titratio
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CHAPTER 6SYNTHESIS AND CHARACTERIZA
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Figure 6.1 Comparison between Fecon
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Figure 6.2 XRD patterns for goethit
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68iron oxide coatings at 60 °C, go
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70substrate diameter of 0.2 mm, an
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72goethite and silica results in on
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Figure 6.7 ESEM micrograph (9000x)
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76Furthermore, because discrete goe
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78Table 6.2 Surface Area and Porosi
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Figure 6.10 Surface charge distribu
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Figure 6.11 Ni adsorption</
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84that for pure silica, and the goe
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Table 7.1 Sample Preparation Condit
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Figure 7.2 EXAFS spectra of Pb/HFO
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Figure 7.3 Fourier transform and fi
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Figure 7.4 Fourier transform and fi
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Table 7.3 EXAFS Results of Pb/HFO S
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967.2 Fe XAS of Iron Oxides and Pb/
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Figure 7.7 EXAFS spectra of iron ox
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100and Venturelli, 1999). Overall t
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102(hematite, goethite, akaganeite,
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104adsorption proc
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106of pH, ionic strength, Pb loadin
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Figure 8.1 Ni adsorption</s
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110high metal load
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Figure 8.3 x(k)•k3 spectra and Fo
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Figure 8.4 (k)•k3 spectra of Ni-H
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Figure 8.5 Fourier transforms (magn
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118be fit using either Fe or Ni ato
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1208.3 EXAFS Analysis of FeThe x(k)
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Table 8.4 EXAFS Results of HFO and
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CHAPTER 9SURFACE COMPLEXATION MODEL
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Figure 9.1 Potentiometric titration
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128Table 9.1 Surface Reactions and
Page 152 and 153:
Page 154 and 155:
132Table 9.2 Model Parameters for N
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Page 158 and 159:
1369.3 Zn Adsorption on GoethiteReg
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Figure 9.6 Zn adsorption</s
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140data over a broad range of condi
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142Figure 9.8 Ni adsorption
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144oxide-coated silica. Ni and Zn s
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Page 170 and 171:
Figure 10.2 Zn adsorption</
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Page 174 and 175:
152one for GACS (2.77x10 -6 mole si
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Figure 10.6 Zn adsorption</
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CHAPTER 11CONCLUSIONS AND FUTURE WO
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158surfaces are needed for successf
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Figure A.2 Ni speciation in 1x10 -5
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Figure A.4 Pb speciation in 5x10 -8
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Figure A.6 Zn speciation in 1x10 -5
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166Table B.2 Potentiometric Titrati
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168Table BA Potentiometric Titratio
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170Table C.3 Zn Adsorption Edges on
Page 194 and 195:
APPENDIX DADSORPTION STUDIES ON SIL
Page 196 and 197:
174Table D.5 Zn Adsorption Isotherm
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176Table E.3 Pb CBC Study on 0.3 g
Page 200 and 201:
APPENDIX GINTRAPARTICLE DIFFUSION M
Page 202 and 203:
180DofA = flier ^ 2fA = Exp(-fD * f
Page 204 and 205:
REFERENCES1. Adamson A. W. (1982) P
Page 206 and 207:
18426. Blake R. L., Hessevick R. E.
Page 208 and 209:
18650. Combes J. M., Manceau A. and
Page 210 and 211:
18876. Elzinga E. J. and Sparks D.
Page 212 and 213:
190102. Gupta V. K. (1998) Equilibr
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192126. Joshi A. and Chaudhuri M. (
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194150. Liu C. and Huang P. M. (200
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196175. Muller B. and Sigg L. (1992
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200. Perry R. H. and Green D. W. (1
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200226. Scheinost A. C., Kretzschma
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202252. Swallow C. K., Hume D. N. a
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204278. Villalobos M., Trotz M. A.
Page 228:
304. Zhong Z. Y., Prozorov T., Feln
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