期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 57, 期 17, 页码 4603-4606出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201800705
关键词
carbon dioxide; electrocatalysis; manganese; N-heterocyclic carbenes; spectroelectrochemistry
资金
- European Commission [ERC-CG-2014-648304]
- ICIQ Foundation
- CELLEX Foundation through the CELLEX-ICIQ high-throughput experimentation platform
- Severo Ochoa Excellence Accreditation [SEV-2013-0319]
- FCT (Portugal) [UID/Multi/04551/2013, RECI/BBB-BQB/0230/2012, PD/BD/105994/2014, IF/00346/2013]
- CELLEX Foundation
- ICIQ Foundation through the CELLEX-ICIQ high-throughput experimentation platform
- Fundação para a Ciência e a Tecnologia [PD/BD/105994/2014] Funding Source: FCT
We report here the first purely organometallic fac-[Mn-I(CO)(3)(bis-(NHC)-N-Me)Br] complex with unprecedented activity for the selective electrocatalytic reduction of CO2 to CO, exceeding 100 turnovers with excellent faradaic yields (eta(CO)approximate to 95%) in anhydrous CH3CN. Under the same conditions, a maximum turnover frequency (TOFmax) of 2100s(-1) was measured by cyclic voltammetry, which clearly exceeds the values reported for other manganese-based catalysts. Moreover, the addition of water leads to the highest TOFmax value (ca. 320000s(-1)) ever reported for a manganese-based catalyst. A Mn-I tetracarbonyl intermediate was detected under catalytic conditions for the first time.
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