Reversible Switching Cu-II/Cu-I Single Sites Catalyze High-rate and Selective CO2 Photoreduction
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作者
Zu, Xiaolong; Zhao, Yuan; Li, Xiaodong; Chen, Runhua; Shao, Weiwei; Li, Li; Qiao, Panzhe; Yan, Wensheng; Pan, Yang; Xu, Qian; Zhu, Junfa; Sun, Yongfu; Xie, Yi
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刊物名称
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
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年、卷、文献号
2022, 62, 1433-7851
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关键词
Zu, Xiaolong; Zhao, Yuan; Li, Xiaodong; Chen, Runhua; Shao, Weiwei; Li, Li; Qiao, Panzhe; Yan, Wensheng; Pan, Yang; Xu, Qian; Zhu, Junfa; Sun, Yongfu; Xie, Yi
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摘要
Herein, we first design a model of reversible redox-switching metal-organic framework single-unit-cell sheets, where the abundant metal single sites benefit for highly selective CO2 reduction, while the reversible redox-switching metal sites can effectively activate CO2 molecules. Taking the synthetic Cu-MOF single-unit-cell sheets as an example, synchrotron-radiation quasi in situ X-ray photoelectron spectra unravel the reversible switching Cu-II/Cu-I single sites initially accept photoexcited electrons and then donate them to CO2 molecules, which favors the rate-liming activation into CO2 delta-, verified by in situ FTIR spectra and Gibbs free energy calculations. As an outcome, Cu-MOF single-unit-cell sheets achieve near 100 % selectivity for CO2 photoreduction to CO with a high rate of 860 mu mol g(-1) h(-1) without any sacrifice reagent or photosensitizer, where both the activity and selectivity outperform previously reported photocatalysts evaluated under similar conditions.
