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复合铁锰硅氧化物催化臭氧化磺胺甲恶唑:吸附与催化反应的协同机制

Catalytic ozonation of sulfamethoxazole by composite iron-manganese silicate oxide: cooperation mechanism between adsorption and catalytic reaction.

作者信息

Gao Guoying, Kang Jing, Shen Jimin, Chen Zhonglin, Chu Wei

机构信息

State Key Laboratory of Urban Water Resource and Environment, School of Municipal & Environmental Engineering, Harbin Institute of Technology, Harbin, 150090, China.

Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong.

出版信息

Environ Sci Pollut Res Int. 2016 Nov;23(21):21360-21368. doi: 10.1007/s11356-016-7376-8. Epub 2016 Aug 9.

Abstract

A systematic investigation of the cooperation mechanism between adsorption and catalytic reaction during the catalytic ozonation of sulfamethoxazole (SMX) by composite iron-manganese silicate oxide (FMSO) was carried out in this work. Results showed that the total organic carbon (TOC) removal increased significantly from 27 % (sole-ozonation) to 79.8 % (FMSO catalytic ozonation). The presence of FMSO in the ozonation process effectively enhanced the ozone utilization efficiency and accelerated the transformation of ozone into hydroxyl radicals. The latter result was verified by the indirect method, using NaHSO as the reductor, and the direct electron spin resonance (ESR) determination technology. The adsorption of SMX on FMSO was minimal (1.8 %). However, ozone rapidly converted SMX into various intermediates, which was exhibited by the much higher adsorption affinity on the surface of FMSO than that of SMX. The accumulation of various intermediates on the FMSO surface also increased their contact probability with the ·OH radicals generated by the ozone decomposition. The continuous interaction of intermediates with ·OH radicals could further promote the benign cycling of the release of adsorption sites and the succeeding adsorption/decomposition of ozone and intermediates on FMSO. This could be another reason for the higher and faster TOC removal rate.

摘要

本研究对复合铁锰硅酸盐氧化物(FMSO)催化臭氧化磺胺甲恶唑(SMX)过程中吸附与催化反应的协同机制进行了系统研究。结果表明,总有机碳(TOC)去除率从单独臭氧化时的27%显著提高至FMSO催化臭氧化时的79.8%。臭氧化过程中FMSO的存在有效提高了臭氧利用效率,并加速了臭氧向羟基自由基的转化。使用NaHSO作为还原剂的间接方法以及直接电子自旋共振(ESR)测定技术验证了后一结果。SMX在FMSO上的吸附量极小(1.8%)。然而,臭氧迅速将SMX转化为各种中间体,这表现为中间体在FMSO表面的吸附亲和力远高于SMX。各种中间体在FMSO表面的积累也增加了它们与臭氧分解产生的·OH自由基的接触概率。中间体与·OH自由基的持续相互作用可进一步促进吸附位点释放以及臭氧和中间体在FMSO上后续吸附/分解的良性循环。这可能是TOC去除率更高且更快的另一个原因。

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