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导致六氢-1,3,5-三硝基-1,3,5-三嗪(RDX)在受污染含水层物质中转化的地球化学和微生物过程。

Geochemical and microbiological processes contributing to the transformation of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) in contaminated aquifer material.

机构信息

Biosciences Division, Argonne National Laboratory, Argonne, IL, United States.

出版信息

Chemosphere. 2011 Aug;84(9):1223-30. doi: 10.1016/j.chemosphere.2011.05.027. Epub 2011 Jun 12.

Abstract

Hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) is a potential human carcinogen, and its contamination of subsurface environments is a significant threat to public health. This study investigated abiotic and biological degradation of RDX in contaminated aquifer material. Anoxic batch systems were started with and without pre-aeration of aquifer material to distinguish initial biological RDX reduction from abiotic RDX reduction. Aerating the sediment eliminated chemical reductants in the native aquifer sediment, primarily Fe(II) sorbed to mineral surfaces. RDX (50 μM) was completely reduced and transformed to ring cleavage products when excess concentrations (2mM) of acetate or lactate were provided as the electron donor for aerated sediment. RDX was reduced concurrently with Fe(III) when acetate was provided, while RDX, Fe(III), and sulfate were reduced simultaneously with lactate amendment. Betaproteobacteria were the dominant microorganisms associated with RDX and Fe(III)/sulfate reduction. In particular, Rhodoferax spp. increased from 21% to 35% and from 28% to 60% after biostimulation by acetate and lactate, respectively. Rarefaction analyses demonstrated that microbial diversity decreased in electron-donor-amended systems with active RDX degradation. Although significant amounts of Fe(III) and/or sulfate were reduced after biostimulation, solid-phase reactive minerals such as magnetite or ferrous sulfides were not observed, suggesting that RDX reduction in the aquifer sediment is due to Fe(II) adsorbed to solid surfaces as a result of Fe(III)-reducing microbial activity. These results suggest that both biotic and abiotic processes play an important role in RDX reduction under in situ conditions.

摘要

六氢-1,3,5-三硝基-1,3,5-三嗪(RDX)是一种潜在的人类致癌物,其对地下环境的污染对公众健康构成了重大威胁。本研究调查了受污染含水层物质中 RDX 的非生物和生物降解。在没有预先对含水层物质进行曝气的情况下,启动了缺氧批量系统,以区分初始生物 RDX 还原和非生物 RDX 还原。对沉积物曝气消除了天然含水层沉积物中的化学还原剂,主要是吸附在矿物表面的 Fe(II)。当提供过量浓度(2mM)的乙酸盐或丙酸盐作为曝气沉积物的电子供体时,RDX(50μM)完全被还原并转化为环裂解产物。当提供乙酸盐时,RDX 与 Fe(III)同时被还原,而当添加丙酸盐时,RDX、Fe(III)和硫酸盐同时被还原。β-变形菌是与 RDX 和 Fe(III)/硫酸盐还原相关的主要微生物。特别是,当分别用乙酸盐和丙酸盐进行生物刺激时,Rhodoferax spp. 从 21%增加到 35%和从 28%增加到 60%。稀疏分析表明,在电子供体添加系统中,随着 RDX 降解的活性增加,微生物多样性降低。尽管在生物刺激后大量的 Fe(III)和/或硫酸盐被还原,但没有观察到固相反应性矿物,如磁铁矿或硫化亚铁,这表明含水层沉积物中的 RDX 还原是由于 Fe(III)-还原微生物活性导致吸附在固体表面的 Fe(II)所致。这些结果表明,在原位条件下,生物和非生物过程都对 RDX 的还原起着重要作用。

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