Yang Tang, Mao Xinnan, Zhang Ying, Wu Xiaoping, Wang Lu, Chu Mingyu, Pao Chih-Wen, Yang Shize, Xu Yong, Huang Xiaoqing
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, China.
Nat Commun. 2021 Oct 15;12(1):6022. doi: 10.1038/s41467-021-26316-6.
CO 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 CN-supported Cu single atom catalysts with tailored coordination structures, namely, Cu-N and Cu-N, can serve as highly selective and active catalysts for CO 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 favors CO hydrogenation to form CHOH via the formate pathway, while Cu-N tends to catalyze CO hydrogenation to produce CO via the reverse water-gas-shift (RWGS) pathway. Significantly, the CHOH productivity and selectivity reach 4.2 mmol g h and 95.5%, respectively, for Cu-N single atom catalyst. We anticipate this work will promote the fundamental researches on the structure-performance relationship of catalysts.
CO加氢反应备受关注，然而，目前催化剂活性低、选择性差以及结构-性能关系不明确等缺点推动了对高效催化剂的探索。我们在此证明，具有定制配位结构的CN负载Cu单原子催化剂，即Cu-N和Cu-N，可以作为低温下CO加氢反应的高选择性和活性催化剂。通过简单改变处理参数就能轻松实现Cu单原子配位结构的调控。进一步研究表明，Cu-N有利于通过甲酸盐途径使CO加氢生成CHOH，而Cu-N则倾向于通过逆水煤气变换（RWGS）途径催化CO加氢生成CO。值得注意的是，对于Cu-N单原子催化剂，CHOH的产率和选择性分别达到4.2 mmol g h和95.5%。我们预计这项工作将推动催化剂结构-性能关系的基础研究。
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