研究了低价态铜分布(Cu⁰/Cu⁺)的铜基催化剂在CO₂加氢制备甲醇中的应用,从低价态铜(Cu、Cu₂O)的催化机理和改进策略等方面展开综述,重点对催化剂上Cu⁰/Cu⁺的反应路径和提高催化性能策略进行了总结,对存在的问题进行了探究。关于在合成甲醇过程中反应的活性位点主要有3个观点,即在Cu⁰-Cu⁺界面上、Cu⁰或Cu⁺上,然而在Cu或Cu₂O表面上加氢制甲醇的最优路径和碳源是不同的。改进策略可以通过改变催化剂表面铜物种的价态分布和保持其价态稳定,以及不同价态铜物种与其他金属氧化物存在密切协同作用2方面进行研究。最后对可控复合价态(Cu⁰/Cu⁺)铜基催化剂做出了预测,并提出可控的复合价态铜基催化剂能够根据碳源和助剂进行选择,为CO₂加氢制甲醇的催化剂研究创造了一个全新的范例。

The application of copper-based catalysts with low valence copper distribution (Cu⁰/Cu⁺) in CO₂ hydrogenation to methanol is studied.The catalytic mechanism and improvement strategies of low valence copper (Cu,Cu₂O) are reviewed,focusing on the reaction pathways of Cu⁰/Cu⁺ on the catalyst and the strategies to improve the catalytic performance.The existing problems are explored.Nowadays,there are three main views on its active sites for the reaction in the synthesis of methanol:at the Cu⁰-Cu⁺ interface,on Cu⁰ or Cu⁺.However,the optimal pathway and carbon source for hydrogenation to methanol on Cu or Cu₂O surface are different.The improvement strategy can be achieved through changing the valence distribution of copper species on the catalyst surface as well as keeping their valence stable,and studying the existence of a close synergy between the low valence Cu species and other metal oxides.The predictions are made for controllable composite valence state (Cu⁰/Cu⁺) Cu-based catalysts,and it is proposed that controllable composite valence state Cu-based catalysts can be selected according to carbon source and additives,creating a new paradigm for catalyst research in CO₂ hydrogenation to methanol.

冼俊杰(1997-),男,硕士生。