Geomicrobiology, Center for Applied Geosciences, University of Tübingen, Hölderlinstr. 12, 72074 Tübingen, Germany.
Environ Sci Technol. 2012 Feb 7;46(3):1439-46. doi: 10.1021/es2016457. Epub 2012 Jan 13.
Green rust (GR) as highly reactive iron mineral potentially plays a key role for the fate of (in)organic contaminants, such as chromium or arsenic, and nitroaromatic compounds functioning both as sorbent and reductant. GR forms as corrosion product of steel but is also naturally present in hydromorphic soils and sediments forming as metastable intermediate during microbial Fe(III) reduction. Although already suggested to form during microbial Fe(II) oxidation, clear evidence for GR formation during microbial Fe(II) oxidation was lacking. In the present study, powder XRD, synchrotron-based XAS, Mössbauer spectroscopy, and TEM demonstrated unambiguously the formation of GR as an intermediate product during Fe(II) oxidation by the nitrate-reducing Fe(II)-oxidizer Acidovorax sp. strain BoFeN1. The spatial distribution and Fe redox-state of the precipitates associated with the cells were visualized by STXM. It showed the presence of extracellular Fe(III), which can be explained by Fe(III) export from the cells or extracellular Fe(II) oxidation by an oxidant diffusing from the cells. Moreover, GR can be oxidized by nitrate/nitrite and is known as a catalyst for oxidation of dissolved Fe(II) by nitrite/nitrate and may thus contribute to the production of extracellular Fe(III). As a result, strain BoFeN1 may contribute to Fe(II) oxidation and nitrate reduction both by an direct enzymatic pathway and an indirect GR-mediated process.
绿锈(GR)作为一种高反应性的铁矿物,可能在铬或砷等无机污染物以及同时作为吸附剂和还原剂的硝基芳香族化合物的命运中起着关键作用。GR 是钢的腐蚀产物,但也存在于水成土壤和沉积物中,在微生物 Fe(III)还原过程中形成亚稳中间体。尽管已经有人提出 GR 在微生物 Fe(II)氧化过程中形成,但缺乏微生物 Fe(II)氧化过程中 GR 形成的明确证据。在本研究中,粉末 XRD、基于同步加速器的 XAS、穆斯堡尔光谱和 TEM 明确证明了硝酸盐还原的 Fe(II)氧化菌 Acidovorax sp. strain BoFeN1 在 Fe(II)氧化过程中形成 GR 作为中间产物。通过 STXM 可视化了与细胞相关的沉淀物的空间分布和 Fe 氧化还原态。结果表明存在细胞外 Fe(III),这可以通过细胞内 Fe(III)的外排或从细胞扩散的氧化剂对细胞外 Fe(II)的氧化来解释。此外,GR 可以被硝酸盐/亚硝酸盐氧化,并且已知是亚硝酸盐/硝酸盐氧化溶解 Fe(II)的催化剂,因此可能有助于细胞外 Fe(III)的产生。因此,BoFeN1 菌株可能通过直接酶促途径和间接的 GR 介导的过程来促进 Fe(II)氧化和硝酸盐还原。