A physical catalyst for the electrolysis of nitrogen to ammonia

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dc.contributor.authorSong, Yangen
dc.contributor.authorJohnson, Danielen
dc.contributor.authorPeng, Ruien
dc.contributor.authorHensley, Dale K.en
dc.contributor.authorBonnesen, Peter V.en
dc.contributor.authorLiang, Liangboen
dc.contributor.authorHuang, Jingsongen
dc.contributor.authorYang, Fengchangen
dc.contributor.authorZhang, Feien
dc.contributor.authorQiao, Ruien
dc.contributor.authorBaddorf, Arthur P.en
dc.contributor.authorTschaplinski, Timothy J.en
dc.contributor.authorEngle, Nancy L.en
dc.contributor.authorHatzell, Marta C.en
dc.contributor.authorWu, Zilien
dc.contributor.authorCullen, David A.en
dc.contributor.authorMeyer, Harry M.en
dc.contributor.authorSumpter, Bobby G.en
dc.contributor.authorRondinone, Adam J.en
dc.date.accessioned2021-11-03T14:27:29Zen
dc.date.available2021-11-03T14:27:29Zen
dc.date.issued2018-04-01en
dc.date.updated2021-11-03T14:27:25Zen
dc.description.abstractAmmonia synthesis consumes 3 to 5% of the world’s natural gas, making it a significant contributor to greenhouse gas emissions. Strategies for synthesizing ammonia that are not dependent on the energy-intensive and methane-based Haber-Bosch process are critically important for reducing global energy consumption and minimizing climate change. Motivated by a need to investigate novel nitrogen fixation mechanisms, we herein describe a highly textured physical catalyst, composed of N-doped carbon nanospikes, that electrochemically reduces dissolved N2 gas to ammonia in an aqueous electrolyte under ambient conditions. The Faradaic efficiency (FE) achieves 11.56 ± 0.85% at −1.19 V versus the reversible hydrogen electrode, and the maximum production rate is 97.18 ± 7.13 mg hour−1 cm−2. The catalyst contains no noble or rare metals but rather has a surface composed of sharp spikes, which concentrates the electric field at the tips, thereby promoting the electroreduction of dissolved N2 molecules near the electrode. The choice of electrolyte is also critically important because the reaction rate is dependent on the counterion type, suggesting a role in enhancing the electric field at the sharp spikes and increasing N2 concentration within the Stern layer. The energy efficiency of the reaction is estimated to be 5.25% at the current FE of 11.56%.en
dc.description.versionPublished versionen
dc.format.extent8 page(s)en
dc.format.mimetypeapplication/pdfen
dc.identifierARTN e1700336 (Article number)en
dc.identifier.doihttps://doi.org/10.1126/sciadv.1700336en
dc.identifier.eissn2375-2548en
dc.identifier.issn2375-2548en
dc.identifier.issue4en
dc.identifier.orcidQiao, Rui [0000-0001-5219-5530]en
dc.identifier.other1700336 (PII)en
dc.identifier.pmid29719860en
dc.identifier.urihttp://hdl.handle.net/10919/106503en
dc.identifier.volume4en
dc.language.isoenen
dc.publisherAAASen
dc.relation.urihttp://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000431374900002&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=930d57c9ac61a043676db62af60056c1en
dc.rightsCreative Commons Attribution-NonCommercial 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by-nc/4.0/en
dc.subjectWORK FUNCTIONen
dc.subjectELECTROCHEMICAL REDUCTIONen
dc.subjectATMOSPHERIC-PRESSUREen
dc.subjectHYDROGEN EVOLUTIONen
dc.subjectEMERSED ELECTRODESen
dc.subjectHIGHLY EFFICIENTen
dc.subjectLOW-TEMPERATUREen
dc.subjectDOPED GRAPHENEen
dc.subjectADSORPTIONen
dc.subjectDINITROGENen
dc.titleA physical catalyst for the electrolysis of nitrogen to ammoniaen
dc.title.serialScience Advancesen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten
dc.type.otherArticleen
dc.type.otherJournalen
dcterms.dateAccepted2018-03-12en
pubs.organisational-group/Virginia Techen
pubs.organisational-group/Virginia Tech/Engineeringen
pubs.organisational-group/Virginia Tech/Engineering/Mechanical Engineeringen
pubs.organisational-group/Virginia Tech/All T&R Facultyen
pubs.organisational-group/Virginia Tech/Engineering/COE T&R Facultyen

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