Статья

Heterogeneous Single‐Atom Catalyst for Visible‐Light‐Driven High‐Turnover CO<sub>2</sub> Reduction: The Role of Electron Transfer

Chao GaoHefei National Laboratory for Physical Sciences at the Microscale iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, and CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230026 P. R. ChinaShuangming ChenHefei National Laboratory for Physical Sciences at the Microscale iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, and CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230026 P. R. ChinaYing WangHefei National Laboratory for Physical Sciences at the Microscale iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, and CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230026 P. R. ChinaJiawen WangHefei National Laboratory for Physical Sciences at the Microscale iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, and CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230026 P. R. ChinaXusheng ZhengHefei National Laboratory for Physical Sciences at the Microscale iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, and CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230026 P. R. ChinaJunfa ZhuHefei National Laboratory for Physical Sciences at the Microscale iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, and CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230026 P. R. ChinaLi SongHefei National Laboratory for Physical Sciences at the Microscale iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, and CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230026 P. R. ChinaWenkai ZhangDepartment of Physics Beijing Normal University Beijing 100875 P. R. ChinaYujie XiongHefei National Laboratory for Physical Sciences at the Microscale iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, and CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230026 P. R. China

2018en

ABI

Аннотация

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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Идентификаторы

DOI: 10.1002/adma.201704624

Цитирования и источники

Цитирований: 2Использованных источников: 0

Показатели — AkademScholar