Topotactic Transformation of Metal-Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts

Li, X; Ao, Z; Liu, J; Sun, H; Rykov, AI; Wang, J

Topotactic Transformation of Metal-Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts

Li, X Ao, Z

Liu, J Sun, H Rykov, AI Wang, J

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Publication Type:: Journal Article
Citation:: ACS Nano, 2016, 10 (12), pp. 11532 - 11540
Issue Date:: 2016-12-27

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Field	Value	Language
dc.contributor.author	Li, X	en_US
dc.contributor.author	Ao, Z https://orcid.org/0000-0003-0333-3727	en_US
dc.contributor.author	Liu, J	en_US
dc.contributor.author	Sun, H	en_US
dc.contributor.author	Rykov, AI	en_US
dc.contributor.author	Wang, J	en_US
dc.date.issued	2016-12-27	en_US
dc.identifier.citation	ACS Nano, 2016, 10 (12), pp. 11532 - 11540	en_US
dc.identifier.issn	1936-0851	en_US
dc.identifier.uri	http://hdl.handle.net/10453/118486
dc.description.abstract	© 2016 American Chemical Society. 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 N2 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.	en_US
dc.relation.ispartof	ACS Nano	en_US
dc.relation.isbasedon	10.1021/acsnano.6b07522	en_US
dc.subject.classification	Nanoscience & Nanotechnology	en_US
dc.title	Topotactic Transformation of Metal-Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts	en_US
dc.type	Journal Article
utslib.citation.volume	12	en_US
utslib.citation.volume	10	en_US
utslib.for	0204 Condensed Matter Physics	en_US
pubs.embargo.period	Not known	en_US
pubs.organisational-group	/University of Technology Sydney
pubs.organisational-group	/University of Technology Sydney/Faculty of Science
pubs.organisational-group	/University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
pubs.organisational-group	/University of Technology Sydney/Strength - CCET - Centre for Clean Energy Technology
utslib.copyright.status	closed_access
pubs.issue	12	en_US
pubs.publication-status	Published	en_US
pubs.volume	10	en_US

Abstract:

© 2016 American Chemical Society. 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 N2 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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http://hdl.handle.net/10453/118486