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纳米零价铁/粘土复合材料上 U(VI)去除机制的光谱和建模研究。

Spectroscopic and modeling investigation of U(VI) removal mechanism on nanoscale zero-valent iron/clay composites.

机构信息

College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, PR China.

College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, PR China.

出版信息

J Colloid Interface Sci. 2023 Jan 15;630(Pt A):395-403. doi: 10.1016/j.jcis.2022.10.008. Epub 2022 Oct 6.

Abstract

Nanoscale zero-valent iron (nZVI)-based composites have been widely utilized in environmental cleanup due to their low cost, high adsorption performance and strong redox activity. Herein, removal mechanism of U(VI) on nZVI/clay composites was demonstrated by batch, XPS and modeling techniques. The batch experiments showed that nZVI/clay composites exhibited the high removal capacity (88.90 mg/g at pH 4.0) and good regeneration towards U(VI) from aqueous solution. The adsorbed U(VI) was mostly reduced to U(IV) by nZVI/clay composites according to XPS analysis. The removal process of U(VI) on nZVI/clay composites was satisfactorily fitted by surface complexation modeling using strong and weak sites, indicating the high chemisorption of U(VI) on nZVI/clay composites. However, the fitting results underestimated U(VI) adsorption at pH 7.0-9.0 due to the reduction of U(VI) into U(IV), whereas the overestimation of U(VI) at pH 4.0-6.0 could be attributed to fewer surface complexation reaction involved. These findings are crucial for the application of nZVI-based composites for the highly efficient removal of radionuclides in actual environmental remediation.

摘要

基于纳米零价铁(nZVI)的复合材料由于其成本低、吸附性能高和强还原活性,已广泛应用于环境净化。本文通过批量实验、XPS 和模型技术,证明了 nZVI/粘土复合材料对 U(VI)的去除机制。批量实验表明,nZVI/粘土复合材料对水溶液中的 U(VI)具有高去除能力(pH4.0 时为 88.90mg/g)和良好的再生性能。XPS 分析表明,吸附的 U(VI)主要被 nZVI/粘土复合材料还原为 U(IV)。U(VI)在 nZVI/粘土复合材料上的去除过程通过强、弱位点的表面络合模型得到了很好的拟合,表明 U(VI)在 nZVI/粘土复合材料上的化学吸附程度较高。然而,由于 U(VI)被还原为 U(IV),在 pH7.0-9.0 时,拟合结果低估了 U(VI)的吸附,而在 pH4.0-6.0 时,过高的拟合结果可能归因于涉及的表面络合反应较少。这些发现对于 nZVI 基复合材料在实际环境修复中高效去除放射性核素的应用至关重要。

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