Journal
ADVANCED MATERIALS
Volume 30, Issue 13, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201704624
Keywords
active sites; carbon dioxide conversion; electron transfer; photocatalysis; single-atom catalysts
Categories
Funding
- National Key R&D Program of China [2017YFA0207301]
- 973 Program [2014CB848900]
- NSFC [21725102, 21471141, U1532135, 21703220]
- CAS Key Research Program of Frontier Sciences [QYZDB-SSW-SLH018]
- CAS Interdisciplinary Innovation Team, Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology [2016FXCX003]
- Recruitment Program of Global Experts, CAS Hundred Talent Program, Anhui Provincial Natural Science Foundation [1708085QB26]
- China Postdoctoral Science Foundation [BH2060000034]
- Fundamental Research Funds for the Central Universities [WK2060190064]
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Visible-light-driven conversion of CO2 into chemical fuels is an intriguing approach to address the energy and environmental challenges. In principle, light harvesting and catalytic reactions can be both optimized by combining the merits of homogeneous and heterogeneous photocatalysts; however, the efficiency of charge transfer between light absorbers and catalytic sites is often too low to limit the overall photocatalytic performance. In this communication, it is reported that the single-atom Co sites coordinated on the partially oxidized graphene nanosheets can serve as a highly active and durable heterogeneous catalyst for CO2 conversion, wherein the graphene bridges homogeneous light absorbers with single-atom catalytic sites for the efficient transfer of photoexcited electrons. As a result, the turnover number for CO production reaches a high value of 678 with an unprecedented turnover frequency of 3.77 min(-1), superior to those obtained with the state-of-theart heterogeneous photocatalysts. This work provides fresh insights into the design of catalytic sites toward photocatalytic CO2 conversion from the angle of single-atom catalysis and highlights the role of charge kinetics in bridging the gap between heterogeneous and homogeneous photocatalysts.
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