Статья

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

Yang TangState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, ChinaXinnan MaoGuangzhou 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, Guangzhou, ChinaYing ZhangState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, ChinaXiaoping WuGuangzhou 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, Guangzhou, ChinaLu WangInstitute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, China. [email protected]Mingyu ChuGuangzhou 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, Guangzhou, ChinaChih‐Wen PaoNational Synchrotron Radiation Research Center, Hsinchu, TaiwanShize YangEyring Materials Center, Arizona State University, Tempe, AZ, USAYong XuGuangzhou 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, Guangzhou, China. [email protected]Xiaoqing HuangState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China. [email protected]

2021en

ABI

Аннотация

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.

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Идентификаторы

DOI: 10.1038/s41467-021-26316-6

Цитирования и источники

Цитирований: 2Использованных источников: 0

Показатели — AkademScholar