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三维分级多孔碳化硅泡沫负载污泥衍生碳作为高效稳定的类芬顿催化剂用于去除恶臭的甲硫醇。

Three-dimensional hierarchical porous sludge-derived carbon supported on silicon carbide foams as effective and stable Fenton-like catalyst for odorous methyl mercaptan elimination.

机构信息

School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, China; Department of Chemistry, National Taiwan University, Taipei 10617, Taiwan.

School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, China.

出版信息

J Hazard Mater. 2018 Sep 15;358:136-144. doi: 10.1016/j.jhazmat.2018.06.045. Epub 2018 Jun 25.

Abstract

The poor reusability of catalysts and secondary pollution are critical issues for sulfur-containing volatile organic compounds (S-VOCs) removal. In this paper, a three-dimensional (3D) hierarchical porous sludge-derived carbon supported on silicon carbide foams (SiC) has been fabricated for deep decomposition of S-VOCs under ambient conditions. The sludge-derived Fenton-like catalyst has been confirmed to be hierarchical 3D porous structure based on detailed characterization by scanning electron microscopy (SEM), X-ray diffraction (XRD), Nitrogen adsorption-desorption measurements and Raman spectroscopy. Significantly, the catalyst after KOH activation (SC-SiC) shows excellent catalytic decomposition of methyl mercaptan (CHSH) with almost complete CHSH oxidation into sulfate using hydrogen peroxide as an oxidant under ambient conditions. This catalyst also possesses relative low iron dissolution and excellent cycling performance. The efficient catalytic ability of SC-SiC can be attributed to SiC foam functioned as a stable 3D macroporous skeleton, in which the porous sludge-derived carbon immobilizes the active iron species and promotes the efficient capture of gaseous CHSH, thus facilitating the decomposition of CHSH by generating reactive species, specifically ·OH. The reaction mechanism was systematically investigated. Herein, the design of the porous sludge-derived carbonaceous Fenton-like catalyst paves an avenue for efficient VOCs treatment and rational sludge disposal.

摘要

催化剂的重复利用率低和二次污染是含硫挥发性有机化合物(S-VOCs)去除的关键问题。在本文中,制备了一种三维(3D)分层多孔碳化硅泡沫负载的污泥衍生碳负载的铁基催化剂(SiC),用于在环境条件下深度分解 S-VOCs。通过扫描电子显微镜(SEM)、X 射线衍射(XRD)、氮气吸附-脱附测量和拉曼光谱等详细表征,证实了污泥衍生的类芬顿催化剂具有分层 3D 多孔结构。值得注意的是,经过 KOH 活化后的催化剂(SC-SiC)在环境条件下使用过氧化氢作为氧化剂,表现出优异的催化分解甲硫醇(CHSH)的性能,几乎可以将 CHSH 完全氧化成硫酸盐。该催化剂还具有相对较低的铁溶出率和优异的循环性能。SC-SiC 的高效催化能力可归因于碳化硅泡沫作为稳定的 3D 大孔骨架的作用,其中多孔的污泥衍生碳固定了活性铁物种,并促进了气态 CHSH 的有效捕获,从而通过生成活性物质,特别是·OH,促进 CHSH 的分解。系统地研究了反应机理。本文中,多孔污泥衍生碳负载的类芬顿催化剂的设计为高效 VOCs 处理和合理的污泥处置开辟了途径。

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