Biomass-derived pyrolytic carbons accelerated Fe(III)/Fe(II) redox cycle for persulfate activation: Pyrolysis temperature-depended performance and mechanisms

被引:71
作者
Liang, Jun [1 ]
Duan, Xiaoguang [2 ]
Xu, Xiaoyun [1 ]
Chen, Kexin [1 ]
Wu, Fei [3 ]
Qiu, Hao [1 ]
Liu, Chengshuai [3 ]
Wang, Shaobin [2 ]
Cao, Xinde [1 ,4 ]
机构
[1] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China
[2] Univ Adelaide, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia
[3] Chinese Acad Sci, Inst Geochem, State Key Lab Environm Geochem, Guiyang 550081, Peoples R China
[4] Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China
基金
国家重点研发计划;
关键词
Pyrolytic carbon; Persulfate; Fe(III); Fe(II) cycle; Fe(IV); Electron transfer; ORGANIC POLLUTANTS; FENTON OXIDATION; FREE-RADICALS; DEGRADATION; BIOCHAR; WATER; TRICHLOROETHYLENE; TRANSFORMATION; REMEDIATION; QUINONES;
D O I
10.1016/j.apcatb.2021.120446
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The oxidation efficiency of iron/persulfate coupled system was limited by the sluggish Fe3+/Fe2+ cycle and severe Fe3+ precipitation. In this study, we reported that pyrolytic carbon under low-temperature (PC400) could significantly and continuously accelerate the Fe3+/Fe2+ circulation in the Fe3+-mediated persulfate system. The fast Fe3+/Fe2+ circulation was due to the transformation between semiquinone radicals and quinones on PC400, resulting in the great reusability and continuous degradation of sulfamethoxazole (SMX). In contrast, pyrolytic carbon derived under high temperature (PC700) could not maintain the Fe3+/Fe2+ cycle for continuous SMX degradation. SMX removal in both two systems was barely affected by the presence of chloride and humic acid. Even in the real water matrixes (e.g., seawater, piggery wastewater, and landfill leachate), appreciable SMX removal was obtained because of the nonradical reaction pathways, including high-valence Fe(IV) and surface electron-transfer process, verified by methyl phenyl sulfoxide-based probe tests, Mo center dot ssbauer spectroscopy, electrochemical test, and kinetic calculation. This study advances the knowledge of Fe3+-mediated persulfate reaction enhanced by pyrolytic carbons. The outcomes will inspire new strategies for developing cost-effective and efficient carbon-accelerated Fenton-like systems.
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页数:10
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