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Single Mo 1 (Cr 1 ) Atom on Nitrogen-Doped Graphene Enables Highly Selective Electroreduction of Nitrogen into Ammonia

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dc.contributor.authorZhao, Wanghui
dc.contributor.authorZhang, Lifu
dc.contributor.authorLuo, Qiquan
dc.contributor.authorHu, Zhenpeng
dc.contributor.authorZhang, Wenhua
dc.contributor.authorSmith, Sean
dc.contributor.authorYang, Jinlong
dc.date.accessioned2020-05-26T23:40:00Z
dc.date.issued2019
dc.date.updated2019-12-19T07:00:07Z
dc.description.abstractSearching for new types of electrocatalysts with high stability, activity, and selectivity is essential for the production of ammonia via electroreduction of nitrogen. Using density functional theory (DFT) calculations, we explore the stability of single metal atoms (M1) supported on nitrogen-doped graphene (N3-G); the competitive adsorption of dinitrogen and hydrogen; and the potential competition of first dinitrogen protonation and hydrogen adsorption on metal sites. Consequently, we identify Mo1/N3-G and Cr1/N3-G as candidate electrocatalysts for nitrogen reduction reaction (NRR). The theoretically predicted selectivities (overpotentials) are 40% (0.34 V) and 100% (0.59 V) on Mo1/N3-G and Cr1/N3-G, respectively. The electroreduction of nitrogen proceeds via distal-to-alternating hybrid mechanism with two spectator dinitrogen molecules. The high stability, high selectivity to ammonia, and relatively low overpotentials for NRR suggest Mo1(Cr1)/N3-G as the most promising electrocatalyst among those studied for electroreduction of nitrogen.en_AU
dc.description.sponsorshipThis work was supported by the National Key Research and Development Program (Grant Nos. 2018YFA0208600, 2016YFA0200600), the National Natural Science Foundation of China (21473167, 21688102, 21703222), the Fundamental Research Funds for the Central Universities (WK3430000005) and partially by the support of China Scholarship Council (CSC) (File No. 201706345015). The calculations were performed on the supercomputing system in USTC-SCC and Guangzhou-SCC.en_AU
dc.format.mimetypeapplication/pdfen_AU
dc.identifier.issn2155-5435en_AU
dc.identifier.urihttp://hdl.handle.net/1885/204675
dc.language.isoen_AUen_AU
dc.publisherAmerican Chemical Societyen_AU
dc.rights© 2019 American Chemical Societyen_AU
dc.sourceACS Catalyisisen_AU
dc.titleSingle Mo 1 (Cr 1 ) Atom on Nitrogen-Doped Graphene Enables Highly Selective Electroreduction of Nitrogen into Ammoniaen_AU
dc.typeJournal articleen_AU
local.bibliographicCitation.issue4en_AU
local.bibliographicCitation.lastpage3425en_AU
local.bibliographicCitation.startpage3419en_AU
local.contributor.affiliationZhao, Wanghui, University of Science and Technology of Chinaen_AU
local.contributor.affiliationZhang, Lifu, Nankai Universityen_AU
local.contributor.affiliationLuo, Qiquan, University of Science and Technology of Chinaen_AU
local.contributor.affiliationHu, Zhenpeng, Nankai Universityen_AU
local.contributor.affiliationZhang, Wenhua, College of Science, ANUen_AU
local.contributor.affiliationSmith, Sean, College of Science, ANUen_AU
local.contributor.affiliationYang, Jinlong, University of Science and Technology of Chinaen_AU
local.contributor.authoremailu1056946@anu.edu.auen_AU
local.contributor.authoruidZhang, Wenhua, t1792en_AU
local.contributor.authoruidSmith, Sean, u1056946en_AU
local.description.embargo2037-12-31
local.description.notesImported from ARIESen_AU
local.identifier.absfor030601 - Catalysis and Mechanisms of Reactionsen_AU
local.identifier.absseo859899 - Environmentally Sustainable Energy Activities not elsewhere classifieden_AU
local.identifier.ariespublicationu3102795xPUB1459en_AU
local.identifier.citationvolume9en_AU
local.identifier.doi10.1021/acscatal.8b05061en_AU
local.identifier.scopusID2-s2.0-85063985456
local.identifier.uidSubmittedByu3102795en_AU
local.publisher.urlhttps://pubs.acs.org/en_AU
local.type.statusPublished Versionen_AU

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