Coordination tailoring of Cu single sites on C3N4 realizes selective CO2 hydrogenation at low temperature

CO 2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by the current disadvantages of poor activity, low selectivity, and ambiguous structure-performance relationship. We demonstrate here that C 3 N 4 -supported Cu single atom catalysts with tailore...

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Veröffentlicht in:	Nature communications Jg. 12; H. 1; S. 6022 - 9
Hauptverfasser:	Yang, Tang, Mao, Xinnan, Zhang, Ying, Wu, Xiaoping, Wang, Lu, Chu, Mingyu, Pao, Chih-Wen, Yang, Shize, Xu, Yong, Huang, Xiaoqing
Format:	Journal Article
Sprache:	Englisch
Veröffentlicht:	London Nature Publishing Group UK 15.10.2021 Nature Publishing Group Nature Portfolio
Schlagworte:	119/118 140/146 147/137 639/301/299 639/638/675 639/638/77/887 Carbon dioxide Carbon nitride Catalysts Coordination Humanities and Social Sciences Hydrogenation Low temperature multidisciplinary Science Science (multidisciplinary) Selectivity Single atom catalysts
ISSN:	2041-1723, 2041-1723
Online-Zugang:	Volltext
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Abstract	CO 2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by the current disadvantages of poor activity, low selectivity, and ambiguous structure-performance relationship. We demonstrate here that C 3 N 4 -supported Cu single atom catalysts with tailored coordination structures, namely, Cu–N 4 and Cu–N 3 , can serve as highly selective and active catalysts for CO 2 hydrogenation at low temperature. The modulation of the coordination structure of Cu single atom is readily realized by simply altering the treatment parameters. Further investigations reveal that Cu–N 4 favors CO 2 hydrogenation to form CH 3 OH via the formate pathway, while Cu–N 3 tends to catalyze CO 2 hydrogenation to produce CO via the reverse water-gas-shift (RWGS) pathway. Significantly, the CH 3 OH productivity and selectivity reach 4.2 mmol g –1 h –1 and 95.5%, respectively, for Cu–N 4 single atom catalyst. We anticipate this work will promote the fundamental researches on the structure-performance relationship of catalysts. CO 2 hydrogenation has attracted intense scientific attention yet suffers from the disadvantage of poor activity and low selectivity. Here, the authors report that Cu single atom catalysts with tailored coordination environments on C 3 N 4 serve as highly selective catalysts for CO 2 hydrogenation.
AbstractList	CO2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by the current disadvantages of poor activity, low selectivity, and ambiguous structure-performance relationship. We demonstrate here that C3N4-supported Cu single atom catalysts with tailored coordination structures, namely, Cu–N4 and Cu–N3, can serve as highly selective and active catalysts for CO2 hydrogenation at low temperature. The modulation of the coordination structure of Cu single atom is readily realized by simply altering the treatment parameters. Further investigations reveal that Cu–N4 favors CO2 hydrogenation to form CH3OH via the formate pathway, while Cu–N3 tends to catalyze CO2 hydrogenation to produce CO via the reverse water-gas-shift (RWGS) pathway. Significantly, the CH3OH productivity and selectivity reach 4.2 mmol g–1 h–1 and 95.5%, respectively, for Cu–N4 single atom catalyst. We anticipate this work will promote the fundamental researches on the structure-performance relationship of catalysts. CO2 hydrogenation has attracted intense scientific attention yet suffers from the disadvantage of poor activity and low selectivity. Here, the authors report that Cu single atom catalysts with tailored coordination environments on C3N4 serve as highly selective catalysts for CO2 hydrogenation. CO 2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by the current disadvantages of poor activity, low selectivity, and ambiguous structure-performance relationship. We demonstrate here that C 3 N 4 -supported Cu single atom catalysts with tailored coordination structures, namely, Cu–N 4 and Cu–N 3 , can serve as highly selective and active catalysts for CO 2 hydrogenation at low temperature. The modulation of the coordination structure of Cu single atom is readily realized by simply altering the treatment parameters. Further investigations reveal that Cu–N 4 favors CO 2 hydrogenation to form CH 3 OH via the formate pathway, while Cu–N 3 tends to catalyze CO 2 hydrogenation to produce CO via the reverse water-gas-shift (RWGS) pathway. Significantly, the CH 3 OH productivity and selectivity reach 4.2 mmol g –1 h –1 and 95.5%, respectively, for Cu–N 4 single atom catalyst. We anticipate this work will promote the fundamental researches on the structure-performance relationship of catalysts. CO 2 hydrogenation has attracted intense scientific attention yet suffers from the disadvantage of poor activity and low selectivity. Here, the authors report that Cu single atom catalysts with tailored coordination environments on C 3 N 4 serve as highly selective catalysts for CO 2 hydrogenation. CO 2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by the current disadvantages of poor activity, low selectivity, and ambiguous structure-performance relationship. We demonstrate here that C 3 N 4 -supported Cu single atom catalysts with tailored coordination structures, namely, Cu–N 4 and Cu–N 3 , can serve as highly selective and active catalysts for CO 2 hydrogenation at low temperature. The modulation of the coordination structure of Cu single atom is readily realized by simply altering the treatment parameters. Further investigations reveal that Cu–N 4 favors CO 2 hydrogenation to form CH 3 OH via the formate pathway, while Cu–N 3 tends to catalyze CO 2 hydrogenation to produce CO via the reverse water-gas-shift (RWGS) pathway. Significantly, the CH 3 OH productivity and selectivity reach 4.2 mmol g –1 h –1 and 95.5%, respectively, for Cu–N 4 single atom catalyst. We anticipate this work will promote the fundamental researches on the structure-performance relationship of catalysts. CO2 hydrogenation has attracted intense scientific attention yet suffers from the disadvantage of poor activity and low selectivity. Here, the authors report that Cu single atom catalysts with tailored coordination environments on C3N4 serve as highly selective catalysts for CO2 hydrogenation. CO2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by the current disadvantages of poor activity, low selectivity, and ambiguous structure-performance relationship. We demonstrate here that C3N4-supported Cu single atom catalysts with tailored coordination structures, namely, Cu-N4 and Cu-N3, can serve as highly selective and active catalysts for CO2 hydrogenation at low temperature. The modulation of the coordination structure of Cu single atom is readily realized by simply altering the treatment parameters. Further investigations reveal that Cu-N4 favors CO2 hydrogenation to form CH3OH via the formate pathway, while Cu-N3 tends to catalyze CO2 hydrogenation to produce CO via the reverse water-gas-shift (RWGS) pathway. Significantly, the CH3OH productivity and selectivity reach 4.2 mmol g-1 h-1 and 95.5%, respectively, for Cu-N4 single atom catalyst. We anticipate this work will promote the fundamental researches on the structure-performance relationship of catalysts.CO2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by the current disadvantages of poor activity, low selectivity, and ambiguous structure-performance relationship. We demonstrate here that C3N4-supported Cu single atom catalysts with tailored coordination structures, namely, Cu-N4 and Cu-N3, can serve as highly selective and active catalysts for CO2 hydrogenation at low temperature. The modulation of the coordination structure of Cu single atom is readily realized by simply altering the treatment parameters. Further investigations reveal that Cu-N4 favors CO2 hydrogenation to form CH3OH via the formate pathway, while Cu-N3 tends to catalyze CO2 hydrogenation to produce CO via the reverse water-gas-shift (RWGS) pathway. Significantly, the CH3OH productivity and selectivity reach 4.2 mmol g-1 h-1 and 95.5%, respectively, for Cu-N4 single atom catalyst. We anticipate this work will promote the fundamental researches on the structure-performance relationship of catalysts.
ArticleNumber	6022
Author	Yang, Tang Pao, Chih-Wen Xu, Yong Mao, Xinnan Wang, Lu Chu, Mingyu Zhang, Ying Huang, Xiaoqing Yang, Shize Wu, Xiaoping
Author_xml	– sequence: 1 givenname: Tang surname: Yang fullname: Yang, Tang organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University – sequence: 2 givenname: Xinnan surname: Mao fullname: Mao, Xinnan organization: Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology – sequence: 3 givenname: Ying surname: Zhang fullname: Zhang, Ying organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University – sequence: 4 givenname: Xiaoping surname: Wu fullname: Wu, Xiaoping organization: Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology – sequence: 5 givenname: Lu orcidid: 0000-0003-0552-1385 surname: Wang fullname: Wang, Lu email: lwang@suda.edu.cn organization: Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University – sequence: 6 givenname: Mingyu surname: Chu fullname: Chu, Mingyu organization: Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology – sequence: 7 givenname: Chih-Wen surname: Pao fullname: Pao, Chih-Wen organization: National Synchrotron Radiation Research Center – sequence: 8 givenname: Shize orcidid: 0000-0002-0421-006X surname: Yang fullname: Yang, Shize organization: Eyring Materials Center, Arizona State University – sequence: 9 givenname: Yong orcidid: 0000-0002-2525-7086 surname: Xu fullname: Xu, Yong email: yongxu@gdut.edu.cn organization: Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology – sequence: 10 givenname: Xiaoqing orcidid: 0000-0003-3219-4316 surname: Huang fullname: Huang, Xiaoqing email: hxq006@xmu.edu.cn organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University
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Snippet	CO 2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by the current disadvantages of poor activity, low... CO2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by the current disadvantages of poor activity, low... CO2 hydrogenation has attracted intense scientific attention yet suffers from the disadvantage of poor activity and low selectivity. Here, the authors report...
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SubjectTerms	119/118 140/146 147/137 639/301/299 639/638/675 639/638/77/887 Carbon dioxide Carbon nitride Catalysts Coordination Humanities and Social Sciences Hydrogenation Low temperature multidisciplinary Science Science (multidisciplinary) Selectivity Single atom catalysts
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Title	Coordination tailoring of Cu single sites on C3N4 realizes selective CO2 hydrogenation at low temperature
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