文献类型：期刊文献

英文题名：Synergy of nitrogen doping and structural defects on hierarchically porous carbons toward catalytic oxidation via a non-radical pathway

作者：Zhang, Wen[1];Li, Yang[1];Fan, Xiaobin[1];Zhang, Fengbao[1];Zhang, Guoliang[1];Zhu, Yi-An[3];Peng, Wenchao[1];Wang, Shaobin[2];Duan, Xiaoguang[2]

机构：[1]Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300350, Peoples R China;[2]Univ Adelaide, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia;[3]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China

年份：2019

卷号：155

起止页码：268

外文期刊名：CARBON

收录：;EI(收录号：20193607395496);WOS:【SCI-EXPANDED(收录号:WOS:000491864400032)】；

基金：This research is supported by project No. 21506158 from the National Natural Science Foundation of China (NSFC). X. D. and S. W. acknowledge the partial support from Open Research Projects of State Key Laboratory (SKL-ChE-16C05 and QAK201808).

语种：英文

外文关键词：Catalyst activity - Activation energy - Biodegradation - Nitrogen - Porous materials - Density functional theory - Design for testability - Rate constants - Doping (additives)

摘要：Engineered carbonaceous materials are promising metal-free catalysts for heterogeneously catalytic oxidation. In this study, hierarchically nitrogen-doped porous carbons are prepared via a one-pot pyrolysis process. The hierarchically porous carbons have a large surface area up to 1641 m(2) g(-1) with a high nitrogen content of 8.63 at.%. The carbons manifested much high catalytic activity in phenol degradation by activation of peroxymonosulfate (PMS) via a non-radical pathway, evidenced by radical screening test, electrochemical measurement and Raman spectra. NZC-S0.5 exhibits outstanding catalytic performance with a turnover frequency (TOF) of 26.0 min(-1). A very high rate constant of 1.3 min(-1) and a small activation energy of 25.1 kJ/mol are achieved. Density functional theory (DFT) calculations illustrate that the most reactive catalytic sites are the N-doped vacancies, confirming the synergetic enhancement by the simultaneously induced heteroatom and structural defects (edges and vacancies). This work enables new insights into heteroatom, structural defects and non-radical pathway in metal-free catalytic PMS activation. (C) 2019 Elsevier Ltd. All rights reserved.