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西番莲壳生物炭主导的单线态氧活化过一硫酸盐用于通过非自由基氧化途径催化降解四环素。

Singlet oxygen-dominated activation of peroxymonosulfate by passion fruit shell derived biochar for catalytic degradation of tetracycline through a non-radical oxidation pathway.

机构信息

National-Local Joint Engineering Research Center of Heavy Metal Pollutant Control and Resource utilization, Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, School of Environmental and Chemical Engineering, Nanchang Hangkong University, Nanchang 330063, China.

National-Local Joint Engineering Research Center of Heavy Metal Pollutant Control and Resource utilization, Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, School of Environmental and Chemical Engineering, Nanchang Hangkong University, Nanchang 330063, China.

出版信息

J Hazard Mater. 2021 Oct 5;419:126495. doi: 10.1016/j.jhazmat.2021.126495. Epub 2021 Jun 25.

DOI:10.1016/j.jhazmat.2021.126495
PMID:34218187
Abstract

Waste-derived biochar has been emerged as promising catalysts to activate peroxymonosulfate (PMS) for the degradation of organic contaminants. Herein, passion fruit shell derived biochar (PFSC) was prepared by a one-pot pyrolysis method and used as a metal-free catalyst to activate PMS for the degradation of tetracycline hydrochloride (TC). The batch experiments indicated that the pyrolysis temperature could influence the efficiency of PFSC for the activation of PMS. In the PFSC-900 (prepared at 900 °C)/PMS system, the degradation rate of TC can reach 90.91%. The quenching test and electron paramagnetic resonance spectra revealed that the high catalytic performance of PFSC-900/PMS system was mainly attributed to the non-free radical reaction pathway containing a carbon bridge, and the TC degradation was controlled primarily by singlet oxygen-mediated oxidation. Moreover, the carboxyl group of ketones and the graphite-N atoms on PFSC-900 are the possible active sites of the non-free radical pathway including direct electron transfer or the formation of O/O. This study not only shows a new type of biochar as an efficient catalyst for PMS activation but also provides a way of value-added reuse of passion fruit shell.

摘要

废基生物炭已被证明是一种很有前途的催化剂,可以激活过一硫酸盐(PMS)来降解有机污染物。在此,采用一步热解法制备了西番莲果壳衍生生物炭(PFSC),并将其用作无金属催化剂来激活过一硫酸盐(PMS)以降解盐酸四环素(TC)。批量实验表明,热解温度会影响 PFSC 对 PMS 的激活效率。在 PFSC-900(在 900°C 下制备)/PMS 体系中,TC 的降解率可达 90.91%。猝灭实验和电子顺磁共振波谱表明,PFSC-900/PMS 体系具有较高的催化性能,主要归因于包含碳桥的非自由基反应途径,且 TC 的降解主要受单线态氧介导的氧化控制。此外,PFSC-900 上酮的羧基和石墨-N 原子可能是包括直接电子转移或 O/O 形成在内的非自由基途径的活性位点。本研究不仅展示了一种新型生物炭作为高效的 PMS 激活催化剂,还为西番莲果壳的增值再利用提供了一种方法。

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