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Fe-Mn 二元氧化物结构和组成对 rGO 去除含水层中 As(III)的影响。

Influence of the structure and composition of Fe-Mn binary oxides on rGO on As(III) removal from aquifers.

机构信息

Key Lab of Groundwater Resources and Environment, Ministry of Education, Jilin University, Changchun 130021, China.

Key Lab of Groundwater Resources and Environment, Ministry of Education, Jilin University, Changchun 130021, China.

出版信息

J Environ Sci (China). 2020 Feb;88:133-144. doi: 10.1016/j.jes.2019.08.008. Epub 2019 Aug 20.

Abstract

Fe-Mn binary oxide (FMBO) possesses high efficiency for As(III) abatement based on the good adsorption affinity of iron oxide and the oxidizing capacity of Mn(IV), and the composition and structure of FMBO play important roles in this process. To compare the removal performance and determine the optimum formula for FMBO, magnetic graphene oxide (MRGO)-FMBO and MRGO-MnO were synthesized with MRGO as a carrier to improve the dispersity of the adsorbents in aquifers and achieve magnetic recycling. Results indicated that MRGO-FMBO had higher As(III) removal than that of MRGO-MnO, although the ratios of Fe and Mn were similar, because the binary oxide of Fe and Mn facilitated electron transfer from Mn(IV) to As(III), while the separation of Mn and Fe on MRGO-MnO restricted the process. The optimal stoichiometry x for MRGO-FMBO (MnFeO) was 0.46, and an extraordinary adsorption capacity of 24.38 mg/g for As(III) was achieved. MRGO-FMBO showed stable dispersive properties in aquifers, and exhibited excellent practicability and reusability, with a saturation magnetization of 7.6 emu/g and high conservation of magnetic properties after 5 cycles of regeneration and reuse. In addition, the presence of coexisting ions would not restrict the practical application of MRGO-FMBO in groundwater remediation. The redox reactions of As(III) and Mn(IV) on MRGO-FMBO were also described. The deprotonated aqueous As(III) on the surface of MRGO-FMBO transferred electrons to Mn(IV), and the formed As(V) oxyanions were bound to ferric oxide as inner-sphere complexes by coordinating their "-OH" groups with Mn(IV) oxides at the surface of MRGO-FMBO. This work could provide new insights into high-performance removal of As(III) in aquifers.

摘要

Fe-Mn 二元氧化物(FMBO)具有高效去除 As(III)的能力,这是基于氧化铁的良好吸附亲和力和 Mn(IV)的氧化能力,而 FMBO 的组成和结构在这个过程中起着重要作用。为了比较去除性能并确定 FMBO 的最佳配方,使用磁性氧化石墨烯(MRGO)作为载体合成了 MRGO-FMBO 和 MRGO-MnO,以提高吸附剂在含水层中的分散性并实现磁性回收。结果表明,尽管 Fe 和 Mn 的比例相似,但 MRGO-FMBO 的 As(III)去除率高于 MRGO-MnO,因为 Fe 和 Mn 的二元氧化物促进了电子从 Mn(IV)向 As(III)的转移,而 MRGO-MnO 上 Mn 和 Fe 的分离限制了这一过程。MRGO-FMBO(MnFeO)的最佳化学计量比 x 为 0.46,对 As(III)的吸附容量达到了 24.38mg/g。MRGO-FMBO 在含水层中表现出稳定的分散性能,具有优异的实用性和可重复使用性,饱和磁化强度为 7.6emu/g,经过 5 次再生和重复使用后,磁性性能保持良好。此外,共存离子的存在不会限制 MRGO-FMBO 在地下水修复中的实际应用。还描述了 MRGO-FMBO 上 As(III)和 Mn(IV)的氧化还原反应。MRGO-FMBO 表面带负电荷的水中 As(III)将电子转移给 Mn(IV),形成的 As(V)含氧阴离子通过与 MRGO-FMBO 表面的 Mn(IV)氧化物的“-OH”基团配位,与氧化铁形成内球络合物。这项工作可以为高效去除含水层中的 As(III)提供新的思路。

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