An EXAFS spectroscopic study of aqueous antimony(III)-chloride complexation at temperatures from 25 to 250°C

Eric H. Oelkers; David M. Sherman; K. Vala Ragnarsdottir; Claire Collins

doi:10.1016/S0009-2541(98)00067-9

An EXAFS spectroscopic study of aqueous antimony(III)-chloride complexation at temperatures from 25 to 250°C

Eric H. Oelkers^*, David M. Sherman, K. Vala Ragnarsdottir, Claire Collins

^*Corresponding author for this work

Faculty of Earth Sciences

Research output: Contribution to journal › Article › peer-review

37 Citations (Scopus)

Abstract

The X-ray adsorption fine structure (EXAFS) spectroscopy of antimony(III)-chloride solutions were obtained at temperatures from 25 to 250°C at pressures corresponding to the liquid-vapor equilibrium curve for H₂O. Two solution compositions were considered: solution A consisted of 0.042 M SbCl₃+2.9 M HCl and solution B consisted of 0.1 M SbCl₃+2.29 M HCl. Interpretation of resulting spectra indicates the presence of aqueous Sb-Cl inner sphere complexes at all investigated temperatures. The average number of chlorine ions in these complexes increases with increasing temperature over the range 25 to 250°C from ∼3.0 to ∼ 3.4 and from ∼2.6 to ∼ 2.9 for solutions A and B, respectively. These results also indicate an increasing average number of chloride ions per complex with increasing aqueous chloride concentration. The Sb-Cl interatomic distances for the two solutions are approximately equal and decrease from 2.42 to 2.38 A with increasing temperature over this range. This latter observation is consistent with theoretical models of aqueous complexation that predict decreasing aqueous species electrostatic radii with increasing temperature.

Original language	English
Pages (from-to)	21-27
Number of pages	7
Journal	Chemical Geology
Volume	151
Issue number	1-4
DOIs	https://doi.org/10.1016/S0009-2541(98)00067-9
Publication status	Published - 1998

Bibliographical note

Funding Information:
We are indebted to Mike Henderson of the University of Manchester for his generous advice, assistance, and encouragement while designing the furnaces and preparing these experiments. Gleb Pokrovski and Eve Valsami-Jones helped run several of the EXAFS spectra. We would like to thank Jacques Schott, Terry Seward, Roy Wogelius, and Eleonora Paris for encouragement and enlightening discussion during the course of this study. The patience and expert advice of Andy Dent, Gert van Dorsen, and Fred Mosselmans, station managers at Daresbury are gratefully acknowledged. Kim George of the glass laboratory at the Department of Biology at Bristol is thanked for sealing the quartz tubes. Finally thanks are also due Fred Wheeler (Bristol) and Claude Lurde (Toulouse) for building and modifying the furnaces used during this study. This study was funded by the CLRC and the Leverhulme Foundation in the U.K., the CNRS in France, and the Deutsche Forschungsgemeinschaft in Germany.

Other keywords

Antimony(III)-chloride solutions
Aqueous complexation
Hydrothermal solutions
X-ray adsorption fine structure (EXAFS) spectroscopy

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10.1016/S0009-2541(98)00067-9

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@article{2393e8a04f164511a0149a80fedbb6c1,

title = "An EXAFS spectroscopic study of aqueous antimony(III)-chloride complexation at temperatures from 25 to 250°C",

abstract = "The X-ray adsorption fine structure (EXAFS) spectroscopy of antimony(III)-chloride solutions were obtained at temperatures from 25 to 250°C at pressures corresponding to the liquid-vapor equilibrium curve for H2O. Two solution compositions were considered: solution A consisted of 0.042 M SbCl3+2.9 M HCl and solution B consisted of 0.1 M SbCl3+2.29 M HCl. Interpretation of resulting spectra indicates the presence of aqueous Sb-Cl inner sphere complexes at all investigated temperatures. The average number of chlorine ions in these complexes increases with increasing temperature over the range 25 to 250°C from ∼3.0 to ∼ 3.4 and from ∼2.6 to ∼ 2.9 for solutions A and B, respectively. These results also indicate an increasing average number of chloride ions per complex with increasing aqueous chloride concentration. The Sb-Cl interatomic distances for the two solutions are approximately equal and decrease from 2.42 to 2.38 A with increasing temperature over this range. This latter observation is consistent with theoretical models of aqueous complexation that predict decreasing aqueous species electrostatic radii with increasing temperature.",

keywords = "Antimony(III)-chloride solutions, Aqueous complexation, Hydrothermal solutions, X-ray adsorption fine structure (EXAFS) spectroscopy",

author = "Oelkers, {Eric H.} and Sherman, {David M.} and Ragnarsdottir, {K. Vala} and Claire Collins",

note = "Funding Information: We are indebted to Mike Henderson of the University of Manchester for his generous advice, assistance, and encouragement while designing the furnaces and preparing these experiments. Gleb Pokrovski and Eve Valsami-Jones helped run several of the EXAFS spectra. We would like to thank Jacques Schott, Terry Seward, Roy Wogelius, and Eleonora Paris for encouragement and enlightening discussion during the course of this study. The patience and expert advice of Andy Dent, Gert van Dorsen, and Fred Mosselmans, station managers at Daresbury are gratefully acknowledged. Kim George of the glass laboratory at the Department of Biology at Bristol is thanked for sealing the quartz tubes. Finally thanks are also due Fred Wheeler (Bristol) and Claude Lurde (Toulouse) for building and modifying the furnaces used during this study. This study was funded by the CLRC and the Leverhulme Foundation in the U.K., the CNRS in France, and the Deutsche Forschungsgemeinschaft in Germany. ",

year = "1998",

doi = "10.1016/S0009-2541(98)00067-9",

language = "English",

volume = "151",

pages = "21--27",

journal = "Chemical Geology",

issn = "0009-2541",

publisher = "Elsevier",

number = "1-4",

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T1 - An EXAFS spectroscopic study of aqueous antimony(III)-chloride complexation at temperatures from 25 to 250°C

AU - Oelkers, Eric H.

AU - Sherman, David M.

AU - Ragnarsdottir, K. Vala

AU - Collins, Claire

N1 - Funding Information: We are indebted to Mike Henderson of the University of Manchester for his generous advice, assistance, and encouragement while designing the furnaces and preparing these experiments. Gleb Pokrovski and Eve Valsami-Jones helped run several of the EXAFS spectra. We would like to thank Jacques Schott, Terry Seward, Roy Wogelius, and Eleonora Paris for encouragement and enlightening discussion during the course of this study. The patience and expert advice of Andy Dent, Gert van Dorsen, and Fred Mosselmans, station managers at Daresbury are gratefully acknowledged. Kim George of the glass laboratory at the Department of Biology at Bristol is thanked for sealing the quartz tubes. Finally thanks are also due Fred Wheeler (Bristol) and Claude Lurde (Toulouse) for building and modifying the furnaces used during this study. This study was funded by the CLRC and the Leverhulme Foundation in the U.K., the CNRS in France, and the Deutsche Forschungsgemeinschaft in Germany.

PY - 1998

Y1 - 1998

N2 - The X-ray adsorption fine structure (EXAFS) spectroscopy of antimony(III)-chloride solutions were obtained at temperatures from 25 to 250°C at pressures corresponding to the liquid-vapor equilibrium curve for H2O. Two solution compositions were considered: solution A consisted of 0.042 M SbCl3+2.9 M HCl and solution B consisted of 0.1 M SbCl3+2.29 M HCl. Interpretation of resulting spectra indicates the presence of aqueous Sb-Cl inner sphere complexes at all investigated temperatures. The average number of chlorine ions in these complexes increases with increasing temperature over the range 25 to 250°C from ∼3.0 to ∼ 3.4 and from ∼2.6 to ∼ 2.9 for solutions A and B, respectively. These results also indicate an increasing average number of chloride ions per complex with increasing aqueous chloride concentration. The Sb-Cl interatomic distances for the two solutions are approximately equal and decrease from 2.42 to 2.38 A with increasing temperature over this range. This latter observation is consistent with theoretical models of aqueous complexation that predict decreasing aqueous species electrostatic radii with increasing temperature.

AB - The X-ray adsorption fine structure (EXAFS) spectroscopy of antimony(III)-chloride solutions were obtained at temperatures from 25 to 250°C at pressures corresponding to the liquid-vapor equilibrium curve for H2O. Two solution compositions were considered: solution A consisted of 0.042 M SbCl3+2.9 M HCl and solution B consisted of 0.1 M SbCl3+2.29 M HCl. Interpretation of resulting spectra indicates the presence of aqueous Sb-Cl inner sphere complexes at all investigated temperatures. The average number of chlorine ions in these complexes increases with increasing temperature over the range 25 to 250°C from ∼3.0 to ∼ 3.4 and from ∼2.6 to ∼ 2.9 for solutions A and B, respectively. These results also indicate an increasing average number of chloride ions per complex with increasing aqueous chloride concentration. The Sb-Cl interatomic distances for the two solutions are approximately equal and decrease from 2.42 to 2.38 A with increasing temperature over this range. This latter observation is consistent with theoretical models of aqueous complexation that predict decreasing aqueous species electrostatic radii with increasing temperature.

KW - Antimony(III)-chloride solutions

KW - Aqueous complexation

KW - Hydrothermal solutions

KW - X-ray adsorption fine structure (EXAFS) spectroscopy

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U2 - 10.1016/S0009-2541(98)00067-9

DO - 10.1016/S0009-2541(98)00067-9

M3 - Article

AN - SCOPUS:0002087580

VL - 151

SP - 21

EP - 27

JO - Chemical Geology

JF - Chemical Geology

SN - 0009-2541

IS - 1-4

ER -

An EXAFS spectroscopic study of aqueous antimony(III)-chloride complexation at temperatures from 25 to 250°C

Abstract

Bibliographical note

Other keywords

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