Hunkeler D, Aravena R
Department of Earth Sciences, University of Waterloo, Waterloo, Ontario, Canada.
Appl Environ Microbiol. 2000 Nov;66(11):4870-6. doi: 10.1128/AEM.66.11.4870-4876.2000.
Carbon isotope fractionation during aerobic mineralization of 1, 2-dichloroethane (1,2-DCA) by Xanthobacter autotrophicus GJ10 was investigated. A strong enrichment of (13)C in residual 1,2-DCA was observed, with a mean fractionation factor alpha +/- standard deviation of 0.968 +/- 0.0013 to 0.973 +/- 0.0015. In addition, a large carbon isotope fractionation between biomass and inorganic carbon occurred. A mechanistic model that links the fractionation factor alpha to the rate constants of the first catabolic enzyme was developed. Based on the model, it was concluded that the strong enrichment of (13)C in 1,2-DCA arises because the first irreversible step of the initial enzymatic transformation of 1,2-DCA consists of an S(N)2 nucleophilic substitution. S(N)2 reactions are accompanied by a large kinetic isotope effect. The substantial carbon isotope fractionation between biomass and inorganic carbon could be explained by the kinetic isotope effect associated with the initial 1,2-DCA transformation and by the metabolic pathway of 1,2-DCA degradation. Carbon isotope fractionation during 1,2-DCA mineralization leads to 1,2-DCA, inorganic carbon, and biomass with characteristic carbon isotope compositions, which may be used to trace the process in contaminated environments.
研究了自养黄色杆菌GJ10对1,2 - 二氯乙烷(1,2 - DCA)进行需氧矿化过程中的碳同位素分馏。观察到残留的1,2 - DCA中(13)C有强烈富集,平均分馏因子α±标准差为0.968±0.0013至0.973±0.0015。此外,生物量与无机碳之间存在较大的碳同位素分馏。建立了一个将分馏因子α与第一种分解代谢酶的速率常数联系起来的机理模型。基于该模型,得出结论:1,2 - DCA中(13)C的强烈富集是因为1,2 - DCA初始酶促转化的第一个不可逆步骤由S(N)2亲核取代组成。S(N)2反应伴随着较大的动力学同位素效应。生物量与无机碳之间大量的碳同位素分馏可以用与1,2 - DCA初始转化相关的动力学同位素效应以及1,2 - DCA降解的代谢途径来解释。1,2 - DCA矿化过程中的碳同位素分馏导致具有特征性碳同位素组成的1,2 - DCA、无机碳和生物量,这可用于追踪污染环境中的该过程。