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源自木材天然纤维素的铁氮共掺杂多孔碳活化过一硫酸盐降解四环素:脱木质素的作用及机制

Iron and nitrogen co-doped porous carbon derived from natural cellulose of wood activating peroxymonosulfate for degradation of tetracycline: Role of delignification and mechanisms.

作者信息

Zheng Kewang, Xiao Ling

机构信息

School of Resource and Environmental Science, Key Laboratory for Biomass-Resource Chemistry and Environmental Biotechnology of Hubei Province, Wuhan University, Wuhan 430072, PR China.

School of Resource and Environmental Science, Key Laboratory for Biomass-Resource Chemistry and Environmental Biotechnology of Hubei Province, Wuhan University, Wuhan 430072, PR China.

出版信息

Int J Biol Macromol. 2022 Dec 1;222(Pt B):2041-2053. doi: 10.1016/j.ijbiomac.2022.10.003. Epub 2022 Oct 7.

Abstract

Iron and nitrogen co-doped porous carbon materials as peroxymonosulfate (PMS) activator for tetracycline (TC) degradation were prepared by pyrolyzing the mixture of iron loading cellulose and melamine under N flow. The cellulose obtained from balsawood through delignification with sodium chlorite. The delignification of wood obviously improved the specific surface area and enhanced the catalytic efficiency of carbon materials obtained after pyrolysis. Enhancing graphitization degree of carbon material demonstrated that delignification of wood was conducive to formation of a short-range ordered graphitic structure during pyrolysis, which facilitated to the improvement of adsorption/catalytic performance of the carbon materials. The prepared catalyst exhibited excellent catalytic stability and adaptability under the conditions of different systems. Radical quenching test and electron paramagnetic resonance measurements suggested that superoxide radical (O·) and singlet oxygen (O) played dominant roles in TC degradation. Fe/FeC, pyridine N and graphite N were the dominant active sites for PMS activation. This research provides new insights for the development of biomass derived high performance carbon catalysts and their application in wastewater treatment via PMS based advanced oxidation processes.

摘要

通过在氮气流下热解负载铁的纤维素和三聚氰胺的混合物,制备了铁和氮共掺杂的多孔碳材料作为过一硫酸盐(PMS)活化剂用于四环素(TC)降解。纤维素是通过用亚氯酸钠对轻木进行脱木质素处理而获得的。木材的脱木质素处理明显提高了比表面积,并增强了热解后所得碳材料的催化效率。提高碳材料的石墨化程度表明,木材的脱木质素处理有利于在热解过程中形成短程有序的石墨结构,这有助于提高碳材料的吸附/催化性能。所制备的催化剂在不同体系条件下表现出优异的催化稳定性和适应性。自由基猝灭试验和电子顺磁共振测量表明,超氧自由基(O·)和单线态氧(O)在TC降解中起主导作用。Fe/FeC、吡啶氮和石墨氮是PMS活化的主要活性位点。该研究为生物质衍生的高性能碳催化剂的开发及其通过基于PMS的高级氧化工艺在废水处理中的应用提供了新的见解。

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