Full metadata record
DC Field | Value | Language |
---|---|---|
dc.contributor.author | 남원우 | * |
dc.contributor.author | Shunichi Fukuzumi | * |
dc.contributor.author | 이용민 | * |
dc.date.accessioned | 2021-06-07T16:31:45Z | - |
dc.date.available | 2021-06-07T16:31:45Z | - |
dc.date.issued | 2021 | * |
dc.identifier.issn | 2155-5435 | * |
dc.identifier.other | OAK-29315 | * |
dc.identifier.uri | https://dspace.ewha.ac.kr/handle/2015.oak/257675 | - |
dc.description.abstract | Selective and efficient catalytic two-electron two-proton (2e(-)/2H(+)) reduction of dioxygen (O-2) to hydrogen peroxide (H2O2) has been achieved less successfully than four-electron four-proton (4e(-)/4H(+)) reduction of O-2 because of the instability of the H2O2 product in the presence of metal catalysts. We report herein a highly efficient 2e(-)/2H(+) reduction of O-2 by ferrocene (Fc; one-electron reductant) and 9,10-dihydro-10-methylacridine (AcrH(2); two-electron reductant and an NADH analog), with a cobalt corrole complex, [Co-III(tpfc)(Py)(2)] (1), in the presence of HClO4 in CH3CN at 298 K, affording a large TON (50,000) and a high turnover frequency (275 s(-1)) with 100% selectivity in producing H2O2. The H2O2 product yielded in the 2e(-)/2H(+) reduction of O-2 using AcrH(2) as a reductant was stable for more than 5 h even in the presence of 1. Detailed kinetic analysis revealed that the rate-determining step (rds) for the 2e(-)/2H(+) reduction of O-2 by Fc with 1 in the presence of HClO4 in CH3CN was the proton-coupled electron transfer from Co-III(tpfc) (2) to O-2 to produce a cobalt(III) corrole radical cation, [CoIII(tpfc(+))](+) (3), which was detected by EPR. When ferrocene was replaced by AcrH(2), the rds became the electron transfer from AcrH(2) to 3, coupled with the deprotonation of AcrH(2)(center dot+) (ET/PT), followed by fast ET from AcrH(center dot) to 3. To the best of our knowledge, this is a report of a highly efficient Co-corrole catalyst that retains its cobalt(III) oxidation state for the 2e(-)/2H(+) reduction of O-2 in producing H2O2 with a high selectivity. | * |
dc.language | English | * |
dc.publisher | AMER CHEMICAL SOC | * |
dc.subject | selective O-2 reduction | * |
dc.subject | cobalt corrole | * |
dc.subject | H2O2 production | * |
dc.subject | reaction mechanism | * |
dc.subject | efficient catalysis | * |
dc.title | Highly Efficient Catalytic Two-Electron Two-Proton Reduction of Dioxygen to Hydrogen Peroxide with a Cobalt Corrole Complex | * |
dc.type | Article | * |
dc.relation.issue | 5 | * |
dc.relation.volume | 11 | * |
dc.relation.index | SCIE | * |
dc.relation.index | SCOPUS | * |
dc.relation.startpage | 3073 | * |
dc.relation.lastpage | 3083 | * |
dc.relation.journaltitle | ACS CATALYSIS | * |
dc.identifier.doi | 10.1021/acscatal.0c05003 | * |
dc.identifier.wosid | WOS:000626844200056 | * |
dc.author.google | Rana, Atanu | * |
dc.author.google | Lee, Yong-Min | * |
dc.author.google | Li, Xialiang | * |
dc.author.google | Cao, Rui | * |
dc.author.google | Fukuzumi, Shunichi | * |
dc.author.google | Nam, Wonwoo | * |
dc.contributor.scopusid | 남원우(7006569723) | * |
dc.contributor.scopusid | Shunichi Fukuzumi(35430038100;58409757400) | * |
dc.contributor.scopusid | 이용민(36546331100;35233855500;57192113229) | * |
dc.date.modifydate | 20240426135715 | * |