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

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ABSTRACTHEAVY METAL ADSORPTION ON IRON OXIDEAND IRON OXIDE-COATED SILICA: MACROSCOPIC, SPECTROSCOPIC,AND MODELING STUDIESbyYing XuTo accurately model <strong>metal</strong> mobility and bioavailability in soils and sediments, systematicsorption studies are needed using representative and well-characterized minerals. Twoimportant surfaces are iron oxide and silica, which are ubiquitous and associated with oneanother in the environment playing important roles in <strong>metal</strong> distribution. The objectivesof this research are to develop models for predicting speciation and mobility of toxictrace <strong>metal</strong> ions in groundwater, soils, and sediments when competing ions are present.A model system for soils and sediments, iron oxide-coated silica, was synthesized; thedegree of coatings was highly sensitive to the particle size of silica and ranged between0.59 and 21.36 mg Fe g-1 solid. The iron oxide coatings increased surface area andintroduced small pores. Surface charge distribution suggested that both silica andgoethite surfaces are important for <strong>adsorption</strong>. The sub-micrometer-sized coatingsexhibited a larger capacity for <strong>metal</strong>s ions than discrete ones and, although in lowconcentration, they greatly affected <strong>metal</strong> affinity to the coated media. X-ray absorptionspectroscopy (XAS) analysis revealed that both Ni(II) and Pb(II) ions form mononuclearbidentate edge-sharing surface complexes on Fe06 octahedra. This mechanism appearedto be invariant of pH, ionic strength, <strong>metal</strong> loading, and reaction time. Constrained withspectroscopic information, the 2-pK triple layer model successfully predicted Ni or Zn<strong>adsorption</strong> in single adsorbate systems. The curvature in <strong>adsorption</strong> isotherms wasaccurately described using two types of sites — high affinity and low affinity ones. A
Page 1: Copyright Warning & RestrictionsThe
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 and 22: LIST OF FIGURES(Continued)FigurePag
Page 23 and 24: CHAPTER 1INTRODUCTIONHeavy<
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
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31• Understand the effect of comp
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33existing in almost all soils and
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CHAPTER 4EXPERIMENTAL METHODSIn thi
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37included coating temperature (T),
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39generated at 45 kV and 40 mA, sca
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41PZC include electrophoretic mobil
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43Lin-edge, from 8,133 to 8,884 eV
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CHAPTER 5CHARACTERIZATION OF IRON O
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47measured by potentiometric titrat
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Table 5.2 XRD Data of Alfa Aesar (A
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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
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174Table D.5 Zn Adsorption Isotherm
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176Table E.3 Pb CBC Study on 0.3 g
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APPENDIX GINTRAPARTICLE DIFFUSION M
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180DofA = flier ^ 2fA = Exp(-fD * f
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REFERENCES1. Adamson A. W. (1982) P
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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
Page 214 and 215:
192126. Joshi A. and Chaudhuri M. (
Page 216 and 217:
194150. Liu C. and Huang P. M. (200
Page 218 and 219:
196175. Muller B. and Sigg L. (1992
Page 220 and 221:
200. Perry R. H. and Green D. W. (1
Page 222 and 223:
200226. Scheinost A. C., Kretzschma
Page 224 and 225:
202252. Swallow C. K., Hume D. N. a
Page 226 and 227:
204278. Villalobos M., Trotz M. A.
Page 228:
304. Zhong Z. Y., Prozorov T., Feln
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