Quantitative X-ray photoelectron spectroscopy-based depth profiling of bioleached arsenopyrite surface by Acidithiobacillus ferrooxidans

Quantitative X-ray photoelectron spectroscopy-based depth profiling of bioleached arsenopyrite surface by Acidithiobacillus ferrooxidans
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基于氧化亚铁硫杆菌生物浸出毒砂表面的定量 X 射线光电子能谱深度分析

DOI:
10.1016/j.gca.2013.11.025
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发表时间:
2014-02
期刊:
Geochemica et Cosmochimica Acta
影响因子:
--
通讯作者:
Rucheng Wang
Rucheng Wang
中科院分区:
其他
文献类型:
--
作者:
Tingting Zhu;Xiancai Lu;Huan Liu;Juan Li;Xiangyu Zhu;Jianjun Lu;Rucheng Wang

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在表生环境中,微生物的活动显著地促进硫化物的氧化并导致重金属的释放,从而造成土壤和沃茨的严重污染。毒砂(FeAsS)是自然界中最常见的砷矿物,是各种环境中的砷污染物。为了研究砷在毒砂微生物氧化过程中的地球化学行为,毒砂切片的(2 - 3 - 0)表面进行了表征后,酸性(pH 2.00)和氧化分解与嗜酸微生物Acidithiobacillusferrooxidans。用扫描电子显微镜和X射线光电子能谱研究了氧化砷黄铁矿表面的形貌、化学和元素深度分布。在细菌的介导下,毒砂表面出现了细胞状和针状的蚀坑,反应10 d后,溶液中砷的释放浓度是非生物反应的50倍。精细尺度XPS深度配置文件的反应毒砂表面后,微生物和非生物氧化的毒砂表面层中的元素的化学状态的变化提供了见解。在450 nm的表面层的非生物氧化的毒砂,Fe(III)-氧化物出现,并逐渐增加向表面,和可检测的亚硫酸盐和一价砷出现在50 nm以上。相比之下,在约3 μm的微生物氧化的毒砂的表面层中发现了较高含量的硫酸铁、亚硫酸盐和亚砷酸盐。中间体,如Fe(III)-AsS和SO,在细菌的存在下是可检测的。XPS深度剖面的氧化态变化表明,在非生物氧化过程中,氧化顺序为Fe > As = S,在微生物氧化过程中,氧化顺序为Fe > S > As。在此基础上,提出了一种可能的微生物氧化反应途径的概念模型。
In supergene environments, microbial activities significantly enhance sulfide oxidation and result in the release of heavy metals, causing serious contamination of soils and waters. As the most commonly encountered arsenic mineral in nature, arsenopyrite (FeAsS) accounts for arsenic contaminants in various environments. In order to investigate the geochemical behavior of arsenic during microbial oxidation of arsenopyrite, (2 3 0) surfaces of arsenopyrite slices were characterized after acidic (pH 2.00) and oxidative decomposition with or without an acidophilic microorganismAcidithiobacillus ferrooxidans. The morphology as well as chemical and elemental depth profiles of the oxidized arsenopyrite surface were investigated by scanning electron microscopy and X-ray photoelectron spectroscopy. With the mediation of bacteria, cell-shaped and acicular pits were observed on the reacted arsenopyrite surface, and the concentration of released arsenic species in solution was 50 times as high as that of the abiotic reaction after 10 days reaction. Fine-scale XPS depth profiles of the reacted arsenopyrite surfaces after both microbial and abiotic oxidation provided insights into the changes in chemical states of the elements in arsenopyrite surface layers. Within the 450 nm surface layer of abiotically oxidized arsenopyrite, Fe(III)-oxides appeared and gradually increased towards the surface, and detectable sulfite and monovalent arsenic appeared above 50 nm. In comparison, higher contents of ferric sulfate, sulfite, and arsenite were found in the surface layer of approximately 3 μm of the microbially oxidized arsenopyrite. Intermediates, such as Fe(III)-AsS and S0, were detectable in the presence of bacteria. Changes of oxidative species derived from XPS depth profiles show the oxidation sequence is Fe > As = S in abiotic oxidation, and Fe > S > As in microbial oxidation. Based on these results, a possible reaction path of microbial oxidation was proposed in a concept model.
不同条件下氧化亚铁硫杆菌生长及附着黄铁矿过程中的基因和蛋白质分析
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