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Topotactic Transformation of Metal-Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts
Li, Xuning1,2; Ao, Zhimin3; Liu, Jiayi1,2; Sun, Hongqi4; Rykov, Alexandre I.1; Wang, Junhu1
KeywordGraphene Encapsulated Mn4n Sulfate Radicals Activation Mechanism Dft Calculation
Source PublicationACS NANO
2016-12-01
DOI10.1021/acsnano.6b07522
Volume10Issue:12Pages:11532-11540
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences ; Technology
WOS SubjectChemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science
WOS KeywordOXYGEN REDUCTION REACTION ; NITROGEN-DOPED GRAPHENE ; BISPHENOL-A ; PEROXYMONOSULFATE ACTIVATION ; HETEROGENEOUS ACTIVATION ; PHENOL DEGRADATION ; NANOPOROUS CARBONS ; AQUEOUS-SOLUTIONS ; SULFATE RADICALS ; FACILE SYNTHESIS
AbstractInnovation 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.
Language英语
WOS IDWOS:000391079700102
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/151851
Collection中国科学院大连化学物理研究所
Affiliation1.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
GB/T 7714
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.
APA Li, Xuning,Ao, Zhimin,Liu, Jiayi,Sun, Hongqi,Rykov, Alexandre I.,&Wang, Junhu.(2016).Topotactic Transformation of Metal-Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts.ACS NANO,10(12),11532-11540.
MLA Li, Xuning,et al."Topotactic Transformation of Metal-Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts".ACS NANO 10.12(2016):11532-11540.
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