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氮、硫和氧共掺杂碳包覆的 Co/CoS 棒(Co/CoS@N-S-O-C)作为过一硫酸盐的高效活化剂用于降解磺胺甲恶唑。

Nitrogen, sulfur and oxygen co-doped carbon-armored Co/CoS rods (Co/CoS@N-S-O-C) as efficient activator of peroxymonosulfate for sulfamethoxazole degradation.

机构信息

Collaborative Innovation Center for Advanced Nuclear Energy Technology, INET, Tsinghua University, Beijing, 100084, PR China; Beijing Key Laboratory of Radioactive Wastes Treatment, Tsinghua University, Beijing, 100084, PR China.

Datang Environment Industry Group Co., Ltd., Beijing, 100097, PR China.

出版信息

J Hazard Mater. 2020 Apr 5;387:121669. doi: 10.1016/j.jhazmat.2019.121669. Epub 2019 Nov 11.

Abstract

In this study, nitrogen, sulfur and oxygen co-doped carbon armored cobalt sulfide (Co/CoS@N-S-O-C) composite was synthesized, characterized and used to activate peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX). SMX (0.04 mM) can be completely degraded within 20 min in the presence of 0.8 mM PMS and 0.1 g/L Co/CoS@N-S-O-C composite. The first-order kinetics constant of SMX degradation was 0.307 min, and the mineralization of SMX was 30.1 %. The Quenching experiments of the free radicals and the identification of degradation products demonstrated that sulfate radicals played a dominant role in SMX degradation. The degradation rate of SMX increased with temperature, and activation energy was calculated to be 48.6 kJ/mol. The degradation rate of SMX increased firstly then decreased with increase of pH. Chloridion and humic acid decreased the degradation rate of SMX no matter what their initial concentration was. The effect of carbonate on SMX degradation depended on its initial concentration. Co/CoS@N-S-O-C composite showed good stability, the removal efficiency of SMX was 98.4 % in the fifth experiment. Based on the characterization results of the catalyst before and after use, it was concluded that cobalt, sulfur, pyridnic N and graphitic N were responsible for PMS activation.

摘要

在这项研究中,合成了氮、硫和氧共掺杂碳铠装钴硫化物(Co/CoS@N-S-O-C)复合材料,并对其进行了表征,用于激活过一硫酸盐(PMS)以降解磺胺甲恶唑(SMX)。在 0.8 mM PMS 和 0.1 g/L Co/CoS@N-S-O-C 复合材料存在下,0.04 mM 的 SMX 可在 20 min 内完全降解。SMX 降解的一级动力学常数为 0.307 min,SMX 的矿化率为 30.1%。自由基淬灭实验和降解产物鉴定表明,硫酸根自由基在 SMX 降解中起主导作用。SMX 的降解速率随温度升高而增加,活化能计算为 48.6 kJ/mol。随着 pH 值的增加,SMX 的降解速率先增加后降低。无论初始浓度如何,氯离子和腐殖酸都会降低 SMX 的降解速率。碳酸盐对 SMX 降解的影响取决于其初始浓度。Co/CoS@N-S-O-C 复合材料表现出良好的稳定性,在第五次实验中,SMX 的去除效率为 98.4%。根据催化剂使用前后的表征结果,推断钴、硫、吡啶氮和石墨氮是 PMS 激活的原因。

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