期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 137, 期 44, 页码 14129-14135出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b08212
关键词
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资金
- Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy (DOE) [DE-AC02-05CH11231]
- BASF SE (Ludwigshafen, Germany)
- King Abdulaziz City of Science and Technology (Riyadh, Saudi Arabia)
- Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, U.S. Department of Energy [DE-AC02-05CH11231]
- U.S. DOE [DE-AC02-05CH11231]
- Suzhou Industrial Park fellowship
- Alexander von Humboldt Foundation
- U.S. Department of Energy (DOE)/Lawrence Berkeley National Laboratory (LBNL) [101528-002]
A key challenge in the field of electrochemical carbon dioxide reduction is the design of catalytic materials featuring high product selectivity, stability, and a composition of earth-abundant elements. In this work, we introduce thin films of nanosized metal organic frameworks (MOFs) as atomically defined and nanoscopic materials that function as catalysts for the efficient and selective reduction of carbon dioxide to carbon monoxide in aqueous electrolytes. Detailed examination of a cobalt porphyrin MOF, Al-2(OH)(2)TCPP-Co (TCPP-H-2 = 4,4',4 '',4 '''-(porphyrin-5,10,15,20-tetrayl)tetrabenzoate) revealed a selectivity for CO production in excess of 76% and stability over 7 h with a per-site turnover number (TON) of 1400. In situ spectroelectrochemical measurements provided insights into the cobalt oxidation state during the course of reaction and showed that the majority of catalytic centers in this MOF are redox-accessible where Co(II) is reduced to Co(I) during catalysis.
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