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题名: Topotactic Transformation of Metal-Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts
作者: Li, Xuning1, 2;  Ao, Zhimin3;  Liu, Jiayi1, 2;  Sun, Hongqi4;  Rykov, Alexandre I.1;  Wang, Junhu1
关键词: graphene encapsulated ;  Mn4N ;  sulfate radicals ;  activation mechanism ;  DFT calculation
刊名: ACS NANO
发表日期: 2016-12-01
DOI: 10.1021/acsnano.6b07522
卷: 10, 期:12, 页:11532-11540
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Multidisciplinary ;  Chemistry, Physical ;  Nanoscience & Nanotechnology ;  Materials Science, Multidisciplinary
研究领域[WOS]: Chemistry ;  Science & Technology - Other Topics ;  Materials Science
英文摘要: 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.
关键词[WOS]: OXYGEN REDUCTION REACTION ;  NITROGEN-DOPED GRAPHENE ;  BISPHENOL-A ;  PEROXYMONOSULFATE ACTIVATION ;  HETEROGENEOUS ACTIVATION ;  PHENOL DEGRADATION ;  NANOPOROUS CARBONS ;  AQUEOUS-SOLUTIONS ;  SULFATE RADICALS ;  FACILE SYNTHESIS
语种: 英语
WOS记录号: WOS:000391079700102
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/151851
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, Mossbauer Effect Data Ctr, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Guangdong Univ Technol, Inst Environm Hlth & Pollut Control, Sch Environm Sci & Engn, Guangzhou 510006, Guangdong, Peoples R China
4.Edith Cowan Univ, Sch Engn, Joondalup, WA 6027, Australia

Recommended Citation:
Li, Xuning,Ao, Zhimin,Liu, Jiayi,et al. Topotactic Transformation of Metal-Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts[J]. ACS NANO,2016,10(12):11532-11540.
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