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

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Mössbauer Effect Data Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
University of Chinese Academy of Sciences, Beijing 100049, China
§ Institute of Environmental Health and Pollution Control, School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou, 510006, China
School of Engineering, Edith Cowan University, Joondalup, Western Australia 6027, Australia
Cite this: ACS Nano 2016, 10, 12, 11532–11540
Publication Date (Web):December 9, 2016
https://doi.org/10.1021/acsnano.6b07522
Copyright © 2016 American Chemical Society
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Abstract

Innovation in transition-metal nitride (TMN) preparation is highly desired for realization of various functionalities. Herein, series of graphene-encapsulated TMNs (FexMn6–xCo4[email protected]) with well-controlled morphology have been synthesized through topotactic transformation of metal–organic frameworks in an N2 atmosphere. The as-synthesized FexMn6–xCo4[email protected] 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[email protected] 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[email protected] was proposed. This study details the insights into versatile TMNs for sustainable remediation by activation of PMS.

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