Evidence of substrate binding and product release via belt-sulfur mobilization of the nitrogenase cofactor
DC Field | Value | Language |
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dc.contributor.author | Lee, Chi Chung | - |
dc.contributor.author | Kang, Wonchull | - |
dc.contributor.author | Jasniewski, Andrew J. | - |
dc.contributor.author | Stiebritz, Martin T. | - |
dc.contributor.author | Tanifuji, Kazuki | - |
dc.contributor.author | Ribbe, Markus W. | - |
dc.contributor.author | Hu, Yilin | - |
dc.date.accessioned | 2022-12-22T01:40:03Z | - |
dc.date.available | 2022-12-22T01:40:03Z | - |
dc.date.created | 2022-12-22 | - |
dc.date.issued | 2022-05 | - |
dc.identifier.issn | 2520-1158 | - |
dc.identifier.uri | http://scholarworks.bwise.kr/ssu/handle/2018.sw.ssu/42942 | - |
dc.description.abstract | Molybdenum nitrogenase catalyses the ambient reduction of N-2 to NH3 at the M-cluster, a complex cofactor that comprises two metal-sulfur partial cubanes ligated by an interstitial carbide and three belt-sulfurs. A recent crystallographic study suggests binding of N-2 via displacement of the belt-sulfur(s) of the M-cluster upon turnover. However, direct proof of N-2 binding and belt-sulfur mobilization during catalysis remains elusive. Here we show that N-2 is captured on the M-cluster via electron and sulfur depletion, and that the N-2-captured state is catalytically competent in generating NH3. Moreover, we demonstrate that product release occurs only when sulfite is supplied along with a reductant, that sulfite is inserted as sulfide into the belt-sulfur-displaced positions and that there is a dynamic in-and-out of belt-sulfurs during catalysis. Together, these results establish the mobilization of cofactor belt-sulfurs as a crucial, yet overlooked, mechanistic element of the nitrogenase reaction. | - |
dc.language | 영어 | - |
dc.language.iso | en | - |
dc.publisher | NATURE PORTFOLIO | - |
dc.relation.isPartOf | NATURE CATALYSIS | - |
dc.title | Evidence of substrate binding and product release via belt-sulfur mobilization of the nitrogenase cofactor | - |
dc.type | Article | - |
dc.identifier.doi | 10.1038/s41929-022-00782-7 | - |
dc.type.rims | ART | - |
dc.identifier.bibliographicCitation | NATURE CATALYSIS, v.5, no.5, pp.443 - 454 | - |
dc.description.journalClass | 1 | - |
dc.identifier.wosid | 000797266800001 | - |
dc.identifier.scopusid | 2-s2.0-85130157303 | - |
dc.citation.endPage | 454 | - |
dc.citation.number | 5 | - |
dc.citation.startPage | 443 | - |
dc.citation.title | NATURE CATALYSIS | - |
dc.citation.volume | 5 | - |
dc.contributor.affiliatedAuthor | Kang, Wonchull | - |
dc.identifier.url | https://www.nature.com/articles/s41929-022-00782-7 | - |
dc.type.docType | Article | - |
dc.description.isOpenAccess | Y | - |
dc.subject.keywordPlus | STEADY-STATE KINETICS | - |
dc.subject.keywordPlus | FEMO-COFACTOR | - |
dc.subject.keywordPlus | AZOTOBACTER-VINELANDII | - |
dc.subject.keywordPlus | N-2 REDUCTION | - |
dc.subject.keywordPlus | HD FORMATION | - |
dc.subject.keywordPlus | MECHANISM | - |
dc.subject.keywordPlus | CARBON | - |
dc.subject.keywordPlus | INTERMEDIATE | - |
dc.subject.keywordPlus | PURIFICATION | - |
dc.subject.keywordPlus | SIMULATION | - |
dc.relation.journalResearchArea | Chemistry | - |
dc.relation.journalWebOfScienceCategory | Chemistry, Physical | - |
dc.description.journalRegisteredClass | scie | - |
dc.description.journalRegisteredClass | scopus | - |
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