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Heterogeneous Single‐Atom Catalyst for Visible‐Light‐Driven High‐Turnover CO 2 Reduction: The Role of Electron Transfer
Author(s) -
Gao Chao,
Chen Shuangming,
Wang Ying,
Wang Jiawen,
Zheng Xusheng,
Zhu Junfa,
Song Li,
Zhang Wenkai,
Xiong Yujie
Publication year - 2018
Publication title -
advanced materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.707
H-Index - 527
eISSN - 1521-4095
pISSN - 0935-9648
DOI - 10.1002/adma.201704624
Subject(s) - catalysis , materials science , photocatalysis , graphene , homogeneous , electron transfer , atom (system on chip) , photochemistry , kinetics , chemical physics , visible spectrum , turnover number , nanotechnology , chemical engineering , optoelectronics , chemistry , thermodynamics , physics , organic chemistry , quantum mechanics , computer science , engineering , embedded system
Abstract Visible‐light‐driven conversion of CO 2 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 CO 2 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‐the‐art heterogeneous photocatalysts. This work provides fresh insights into the design of catalytic sites toward photocatalytic CO 2 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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