Two-stage chromium isotope fractionation during microbial Cr(VI) reduction

分馏 同位素分馏 平衡分馏 化学 质量无关分馏 舍瓦内拉 同位素 稳定同位素比值 环境化学 色谱法 地质学 有机化学 细菌 古生物学 物理 量子力学
作者
Guojun Chen,Jun-Cheng Han,Yang Mu,Haiying Yu,Liping Qin
出处
期刊:Water Research [Elsevier BV]
卷期号:148: 10-18 被引量:46
标识
DOI:10.1016/j.watres.2018.09.034
摘要

Chromium isotope fractionation analysis is a promising approach for the assessment of microbial Cr(VI) reduction in groundwater. Understanding the mechanisms and other parameters that control Cr isotope fractionation factors (between the product Cr(III) and reactant Cr (VI)) in microbial Cr(VI) reduction is critical to this application. To date, such studies are very limited. Here, the influence of critical factors on observed Cr isotope fractionation during Cr(VI) reduction by Shewanella oneidensis MR-1 under various conditions was investigated. The Cr(VI) concentration and Cr isotope ratio measurements were conducted on unreacted Cr(VI) remaining in solution to determine Cr isotope fractionation factors. The changes in ambient environmental conditions (e.g., pH, temperature) have limited influence on Cr isotope fractionation factors. However, as a result of Cr(VI) consumption as the experiments proceed, the change in bioavailability of Cr(VI) has a significant impact on Cr isotope fractionation factors. For example, in temperature-controlled experiments, Cr isotope fractionation showed two-stage behavior: during Stage I, the values of ε were −2.81 ± 0.19‰ and −2.60 ± 0.14‰ at 18 °C and 34 °C, respectively; during Stage II, as Cr(VI) reduction progressed, Cr isotope fractionation was significantly masked, and the ε values decreased to −0.98 ± 0.49‰ and −1.01 ± 0.11‰ at 18 °C and 34 °C, respectively. Similar two-stage isotope fractionation behaviors were observed in pH-controlled experiments (pH = 6.0 and 7.2) and in experiments with and without the addition of a competing electron acceptor (nitrate). Masking of isotope fractionation in Stage II indicated restrictions on the bioavailability of Cr(VI) and mass-transfer limitations. This study provides an explanation for the variation in Cr isotope fractionation factors during microbial Cr(VI) reduction in the environment, furthering the viability of Cr isotope ratio analysis as an approach in understanding Cr biogeochemical cycling.
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