期刊
ACS NANO
卷 10, 期 12, 页码 11532-11540出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.6b07522
关键词
graphene encapsulated; Mn4N; sulfate radicals; activation mechanism; DFT calculation
类别
资金
- National Natural Science Foundation of China [21476232, 21607029]
- Chinese Academy of Sciences Visiting Professorships for Senior International Scientists [2011T1G15]
- 1000 plan for Young Professionals Program of China
- 100 Talents Program of Guangdong University of Technology
Innovation in transition-metal nitride (TMN) preparation is highly desired for realization of various functionalities. Herein, series of graphene-encapsulated TMNs (FexMn6-xCo4-N@C) with well-controlled morphology have been synthesized through topotactic transformation of metal-organic frameworks in an N-2 atmosphere. The as-synthesized FexMn6-xCo4-N@C nanodices were systematically characterized and functionalized as Fenton-like catalysts for catalytic bisphenol A (BPA) oxidation by activation of peroxymonosulfate (PMS). The catalytic performance of FexMn6-xCo4-N@C was found to be largely enhanced with increasing Mn content. Theoretical calculations illustrated that the dramatically reduced adsorption energy and facilitated electron transfer for PMS activation catalyzed by Mn4N are the main factors for the excellent activity. Both sulfate and hydroxyl radicals were identified during the PMS activation, and the BPA degradation pathway mainly through hydroxylation, oxidation, and decarboxylation was investigated. Based on the systematic characterization of the catalyst before and after the reaction, the overall PMS activation mechanism over FexMn6-xCo4-N@C was proposed. This study details the insights into versatile TMNs for sustainable remediation by activation of PMS.
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