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Gallium isotope fractionation during Ga adsorption on calcite and goethite
Wei Yuan;  Giuseppe D.Saldi;  JiuBin Chen;  MarinoVetuschi Zuccolini;  Jean-Louis Birck;  Yujie Liu;  Jacques Schott
2018
发表期刊Geochimica et Cosmochimica Acta
卷号223页码:350-363
摘要

Gallium (Ga) isotopic fractionation during its adsorption on calcite and goethite was investigated at 20 °C as a function of the solution pH, Ga aqueous concentration and speciation, and the solid to solution ratio. In all experiments Ga was found to be enriched in light isotopes at the solid surface with isotope fractionation △71Gasolid-solution up to −1.27‰ and −0.89‰ for calcite and goethite, respectively. Comparison of Ga isotopic data of this study with predictions for ‘closed system’ equilibrium and ‘Rayleigh fractionation’ models indicates that the experimental data are consistent with a ‘closed system’ equilibrium exchange between the fluid and the solid. The results of this study can be interpreted based on Ga aqueous speciation and the structure of Ga complexes formed at the solid surfaces. For calcite, Ga isotope fractionation is mainly triggered by increased Ga coordination and Ga–O bond length, which vary respectively from 4 and 1.84 Å in Ga(OH)4 to 6 and 1.94 Å in the >Ca–O–GaOH(OH2)4+ surface complex. For goethite, despite the formation of Ga hexa-coordinated >FeOGa(OH)20 surface complexes (Ga–O distances of 1.96–1.98 Å) both at acid and alkaline pH, a similar extent of isotope fractionation was found at acid and alkaline pH, suggesting that Ga(OH)4 is preferentially adsorbed on goethite for all investigated pH conditions. In addition, the observed decrease of Ga isotope fractionation magnitude observed with increasing Ga surface coverage for both calcite and goethite is likely related to the formation of Ga surface polymers and/or hydroxides with reduced Ga–O distances. This first study of Ga isotope fractionation during solid-fluid interactions suggests that the adsorption of Ga by oxides, carbonates or clay minerals could yield significant Ga isotope fractionation between secondary minerals and surficial fluids including seawater. Ga isotopes thus should help to better characterize the surficial biogeochemical cycles of gallium and its geochemical analog aluminum.

关键词Gallium Isotopes Significant Fractionation Adsorption Calcite Goethite
收录类别SCI
语种英语
文献类型期刊论文
条目标识符http://ir.gyig.ac.cn/handle/42920512-1/8415
专题环境地球化学国家重点实验室
作者单位1.State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550081, China
2.University of Chinese Academy of Sciences, Beijing 100049, China
3.Ge´oscience Environnement Toulouse, CNRS (UMP 5563)-OMP-Universite´ Paul-Sabatier, 14, Avenue E´ douard Belin, 31400 Toulouse, France
4.Laboratorio di Geochimica at DIPTERIS, Universita` di Genova, Corso Europa 26, 16132 Genova, Italy
5.Laboratoire de Geochimie et Cosmochimie, Institute de Physique du Globe de Paris (IPGP), 75252 Paris, France
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Wei Yuan;Giuseppe D.Saldi;JiuBin Chen;MarinoVetuschi Zuccolini;Jean-Louis Birck;Yujie Liu;Jacques Schott. Gallium isotope fractionation during Ga adsorption on calcite and goethite[J]. Geochimica et Cosmochimica Acta,2018,223:350-363.
APA Wei Yuan;Giuseppe D.Saldi;JiuBin Chen;MarinoVetuschi Zuccolini;Jean-Louis Birck;Yujie Liu;Jacques Schott.(2018).Gallium isotope fractionation during Ga adsorption on calcite and goethite.Geochimica et Cosmochimica Acta,223,350-363.
MLA Wei Yuan;Giuseppe D.Saldi;JiuBin Chen;MarinoVetuschi Zuccolini;Jean-Louis Birck;Yujie Liu;Jacques Schott."Gallium isotope fractionation during Ga adsorption on calcite and goethite".Geochimica et Cosmochimica Acta 223(2018):350-363.
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