DC Field | Value | Language |
---|---|---|
dc.contributor.author | Shin, Dongyup | ko |
dc.contributor.author | Choi, Hansol | ko |
dc.contributor.author | An, Jihun | ko |
dc.contributor.author | Sohn, Chang Ho | ko |
dc.contributor.author | Choi, Chang Hyuck | ko |
dc.contributor.author | Shin, Hyeyoung | ko |
dc.contributor.author | Kim, Hyungjun | ko |
dc.date.accessioned | 2022-11-10T03:00:34Z | - |
dc.date.available | 2022-11-10T03:00:34Z | - |
dc.date.created | 2022-11-01 | - |
dc.date.created | 2022-11-01 | - |
dc.date.created | 2022-11-01 | - |
dc.date.created | 2022-11-01 | - |
dc.date.created | 2022-11-01 | - |
dc.date.issued | 2022-11 | - |
dc.identifier.citation | JOURNAL OF MATERIALS CHEMISTRY A, v.10, no.42, pp.22523 - 22530 | - |
dc.identifier.issn | 2050-7488 | - |
dc.identifier.uri | http://hdl.handle.net/10203/299456 | - |
dc.description.abstract | Many studies have focused on atomically dispersed metal-nitrogen-carbon (Me-N-C) catalysts owing to their unique chemistry and high catalytic activities. Me-N-C catalysts have active centers resembling metalloporphyrins; thus, being heterogeneous analogs of homogeneous catalysts, their catalytic characteristics can be described by organometallic principles. In this regard, the high electrochemical activity of Ni-N-C catalysts for carbon dioxide reduction reactions (CO(2)RRs) is particularly difficult to understand because Ni2+ is a d(8) species with a chemically inert axial site for intermediate binding in a square-planar ligand field. To resolve such a conundrum, we investigated the effects of different coordination geometries and Ni spin states on CO2RR activities-both of which influence the chemical activity of the Ni center. We used the grand-canonical density functional theory (GC-DFT) and the occupation matrix control method to properly include a finite potential effect, and to control the oxidation state of the Ni center, respectively. We elucidated that the generation of Ni+ directly impacts the CO2RR activity by providing strong intermediate binding energies to the Ni center, and a defective coordination environment is essential for stabilizing the Ni+ oxidation state. Our present study identifying governing factors for the high catalytic activity of Ni-N-C catalysts provides a design principle to develop high-performing catalysts for CO2RR. | - |
dc.language | English | - |
dc.publisher | ROYAL SOC CHEMISTRY | - |
dc.title | Enhanced electroreduction of CO2 by Ni-N-C catalysts from the interplay between valency and local coordination symmetry | - |
dc.type | Article | - |
dc.identifier.wosid | 000870366500001 | - |
dc.identifier.scopusid | 2-s2.0-85141032370 | - |
dc.type.rims | ART | - |
dc.citation.volume | 10 | - |
dc.citation.issue | 42 | - |
dc.citation.beginningpage | 22523 | - |
dc.citation.endingpage | 22530 | - |
dc.citation.publicationname | JOURNAL OF MATERIALS CHEMISTRY A | - |
dc.identifier.doi | 10.1039/d2ta05844h | - |
dc.contributor.localauthor | Sohn, Chang Ho | - |
dc.contributor.localauthor | Kim, Hyungjun | - |
dc.contributor.nonIdAuthor | Choi, Hansol | - |
dc.contributor.nonIdAuthor | Choi, Chang Hyuck | - |
dc.contributor.nonIdAuthor | Shin, Hyeyoung | - |
dc.description.isOpenAccess | N | - |
dc.type.journalArticle | Article | - |
dc.subject.keywordPlus | ELECTROCHEMICAL REDUCTION | - |
dc.subject.keywordPlus | CARBON NANOTUBES | - |
dc.subject.keywordPlus | METAL | - |
dc.subject.keywordPlus | CONVERSION | - |
dc.subject.keywordPlus | GRAPHENE | - |
dc.subject.keywordPlus | IDENTIFICATION | - |
dc.subject.keywordPlus | ATOMS | - |
dc.subject.keywordPlus | GOLD | - |
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