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钴镍粉复合催化剂协同过一硫酸盐降解磺胺甲恶唑:性能、降解途径及机理探讨。

Degradation of sulfamethoxazole by cobalt-nickel powder composite catalyst coupled with peroxymonosulfate: Performance, degradation pathways and mechanistic consideration.

机构信息

State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu, 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu, 610065, China.

Laboratory of Wastewater Treatment Technology in Sichuan Province, Haitian Water Group, China.

出版信息

J Hazard Mater. 2020 Dec 5;400:123322. doi: 10.1016/j.jhazmat.2020.123322. Epub 2020 Jun 26.

DOI:10.1016/j.jhazmat.2020.123322
PMID:32947719
Abstract

In this work, cobalt-nickel powder (Co-NP) synthesized through electroless plating was used as a heterogeneous bimetallic catalyst for peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX) in the aqueous phase. Compared with different oxidation systems and different catalysts, it was proved that Co-NP had excellent catalytic ability, fast electron transfer rate and good stability. The effects of key parameters (initial pH, SMX concentration, catalyst and PMS dosages) on SMX degradation and ion leaching were studied in detail. Furthermore, the sensitivity of inorganic anions and different pollutants towards the Co-NP/PMS system was studied to investigate its application in natural water bodies. Quenching test showed that the main reactive oxygen species generated during the reaction were OH and SO, of which SO played a predominating role. Combined with XPS analysis, the activation mechanism was concluded that free radicals were mainly generated through the valence change of Co and Ni. Based on the seven intermediates measured through ultrahigh performance liquid chromatograph-mass spectrometry (UPLC-QTOF-MS/MS), the possible degradation pathways of SMX were proposed. Notably, this study provided a new kind of supporter for advanced oxidation processes and electroless plating technology.

摘要

在这项工作中,通过化学镀合成的钴镍粉末(Co-NP)被用作多相双金属催化剂,用于活化过一硫酸盐(PMS)以降解水相中磺胺甲恶唑(SMX)。与不同的氧化体系和不同的催化剂相比,证明 Co-NP 具有优异的催化能力、快速的电子转移速率和良好的稳定性。详细研究了关键参数(初始 pH 值、SMX 浓度、催化剂和 PMS 剂量)对 SMX 降解和离子浸出的影响。此外,还研究了无机阴离子和不同污染物对 Co-NP/PMS 体系的敏感性,以考察其在天然水体中的应用。猝灭试验表明,反应过程中产生的主要活性氧物质是 OH 和 SO ,其中 SO 起主导作用。结合 XPS 分析,得出的活化机制是自由基主要通过 Co 和 Ni 的价态变化产生。根据通过超高效液相色谱-飞行时间质谱(UPLC-QTOF-MS/MS)测量的 7 种中间体,提出了 SMX 的可能降解途径。值得注意的是,本研究为高级氧化工艺和化学镀技术提供了一种新的载体。

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