α-氧化铝-细菌二元复合胶体对锑的吸附研究
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S153

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国家自然科学基金项目(41907015)和湖南省教育厅优秀青年基金项目(18B120)资助


Adsorption of Antimony by α-Al2O3-bacteria Binary Composite Colloid
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Supported by the National Natural Science Foundation of China (No. 41907015) and the Scientific Research Fund of Hunan Provincial Education Department, China (No. 18B120)

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    摘要:

    锑(Sb)在土壤胶体微界面的吸附解吸深刻影响其迁移、转化和归趋。土壤矿物、有机物、微生物等胶体组分多结合在一起,形成复杂的矿物-有机复合体。目前,锑在单一土壤组分上的吸附研究颇多,但较少有学者关注锑在土壤矿物-有机复合胶体界面的吸附过程和机制。通过宏观吸附以及光谱学技术探究锑在典型铝氧化物-细菌复合胶体上的吸附行为,结果表明:α-Al2O3纳米级颗粒覆盖在蜡状芽孢杆菌表面,形成一层不完整的“矿物膜”。朗格缪尔(Langmuir)模型可以很好地拟合Sb(V,Ⅲ)的等温吸附数据(R2>0.98);α-Al2O3对Sb的吸附量远大于细菌;Sb在Al2O3-细菌复合胶体上的吸附不符合“组分相加”原则,存在显著的促进效应。扫描电镜-能谱分析显示Sb主要结合在复合胶体的矿物组分上。X-射线光电子能谱结果表明铝羟基、羧基和氨基参与了Sb的吸附,且细菌会抑制Sb(Ⅲ)在α-Al2O3表面的氧化。本研究证实,细菌不仅影响锑在矿物界面的吸附量,还影响其氧化还原反应,因此,在预测锑在土壤中的形态转化、迁移和归趋时必须考虑矿物-微生物相互作用。

    Abstract:

    [Objective] Adsorption-desorption of Sb on micro-interfaces of soil colloids deeply affects its mobility, transformation and fate in the soil environment. Various soil minerals, organic matter (OM), microbes and soil colloids often combine with each other to form complicated mineral-organic complexes, which vary in properties (e.g., surface charge, particle size and the functional groups) with their composition and hence affect adsorption-desorption of the trace element differently. So far, though much have been done on the behaviors of antimony binding to single soil components, little attention has been paid to adsorption processes of Sb to mineral-organic composites and its mechanism.[Method] In this study, a batch adsorption experiment was carried out to investigate Sb (V/Ⅲ) adsorption behaviors on the interfaces of typical aluminum oxide-bacteria composites different in component ratio (30:70 and 70:30), with the aid of spectroscopic techniques and to validate whether bacteria affect Sb oxidation on mineral surfaces and to explore underlying mechanisms.[Result] Nano-sized particles of α-Al2O3 over on the surface of Bacillus cereus form an incomplete "mineral film", which may suggest that some of the available adsorption sites on either the mineral or the bacterial cells are covered or blocked. The Langmuir model can adequately describe Sb adsorption isotherms with a goodness of R2>0.98; α-Al2O3 adsorbs much more Sb (~50 mg·g-1) than bacterial cells(15-24 mg·g-1), which may be explained by difference in surface charge property, i.e., bacteria are negatively charged whereas α-Al2O3 is positively charged; the binding of Sb to α-Al2O3-bacteria composites does not follow the "component additive rule", i.e., the sum of the individual adsorptivities, but is significantly enhanced compared to the predicted assuming additivity. Scanning electron microscopy-energy spectrum analysis shows that the elemental distribution of Sb is highly correlated to that of Al rather than C, suggesting that Sb is mostly bound to minerals in the binary composites; and XPS analysis shows that the AlOH group of α-Al2O3 and the COOH and NH2 groups of bacteria are all involved in binding Sb in the binary composite, possibly through formation of strong inner-sphere type complexes; moreover, bacteria inhibit oxidation of Sb (Ⅲ) on the surface of α-Al2O3, probably indirectly by hindering electron transfer between Sb and α-Al2O3.[Conclusion] All the findings in the study suggest that bacteria affect not only the quantity of Sb adsorbed onto Al minerals, but also oxidation-reduction of the element, therefore mineral-organic interaction should be taken into account in predicting transformation, translocation and fate of antimony in soils.

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杜辉辉,陶洁,聂宁,雷鸣,杨蕊嘉,铁柏清.α-氧化铝-细菌二元复合胶体对锑的吸附研究[J].土壤学报,2021,58(3):704-711. DOI:10.11766/trxb201911080492 DU Huihui, TAO Jie, NIE Ning, LEI Ming, YANG Ruijia, TIE Boqing. Adsorption of Antimony by α-Al2O3-bacteria Binary Composite Colloid[J]. Acta Pedologica Sinica,2021,58(3):704-711.

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  • 收稿日期:2019-11-08
  • 最后修改日期:2020-03-05
  • 录用日期:2020-03-31
  • 在线发布日期: 2020-12-10
  • 出版日期: 2021-05-11