Zinc Isotope Fractionation during Sorption onto Al Oxides: Atomic Level Understanding from EXAFS

Environmental Science & Technology
Wenxian GouWeiqiang Li

Abstract

Interactions between aqueous Zn and mineral surfaces can lead to notable Zn isotope fractionation that affects Zn source fingerprinting, which needs an atomic-level understanding. In this study, we demonstrate that Zn isotope fractionation (Δ66Znsorbed-aqueous) during Zn sorption onto γ-Al2O3 depends on both pH and Zn concentration and ultimately correlates to surface coverage (Γ). At pH values of 6.0-6.5 and/or Zn concentrations of 0.1-0.2 mM, where Γ < 0.8 μmol m-2, Δ66Znsorbed-solution is 0.47 ± 0.03‰, whereas Δ66Znsorbed-aqueous decreases to 0.02 ± 0.07‰ at pH values of 7.0-8.0 and Zn concentrations of 0.4-0.8 mM, with a high Γ ranging from 1.5 to 3.2 μmol m-2. Using extended X-ray absorption fine structure (EXAFS) spectroscopy, we elucidated that a Zn-Al layered double hydroxide (LDH) with a Zn-O bond length of 2.06 Å forms at high surface coverage (1.5 < Γ < 3.2 μmol m-2). In contrast, at low surface coverage (Γ < 0.8 μmol m-2), the sorbed Zn occurs as a tetrahedrally coordinated inner-sphere surface complex with an average Zn-O interatomic distance of 1.98 Å. Such contrasts lead to an atomic level understanding of the strong links between isotope fractionation, local bonding structures (i.e., coordination and bond distan...Continue Reading

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Citations

Jun 24, 2020·The Science of the Total Environment·Anne-Marie Desaulty, Emmanuelle Petelet-Giraud
Aug 10, 2021·Environmental Science & Technology·Xinran YanHui Yin
Feb 29, 2020·Analytical Chemistry·Kang ShuaiHejiu Hui
Jan 24, 2022·The Science of the Total Environment·Bin LiangYe Zhao

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