Chai Yuchao, Qin Bin, Li Bonan, Dai Weili, Wu Guangjun, Guan Naijia, Li Landong
Key Laboratory of Advanced Energy Materials Chemistry of Ministry of Education, College of Chemistry, Nankai University, Tianjin 300071, China.
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Natl Sci Rev. 2023 Feb 20;10(7):nwad043. doi: 10.1093/nsr/nwad043. eCollection 2023 Jul.
The selective hydrogenation of CO to methanol by renewable hydrogen source represents an attractive route for CO recycling and is carbon neutral. Stable catalysts with high activity and methanol selectivity are being vigorously pursued, and current debates on the active site and reaction pathway need to be clarified. Here, we report a design of faujasite-encaged mononuclear Cu centers, namely Cu@FAU, for this challenging reaction. Stable methanol space-time-yield (STY) of 12.8 mmol g h and methanol selectivity of 89.5% are simultaneously achieved at a relatively low reaction temperature of 513 K, making Cu@FAU a potential methanol synthesis catalyst from CO hydrogenation. With zeolite-encaged mononuclear Cu centers as the destined active sites, the unique reaction pathway of stepwise CO hydrogenation over Cu@FAU is illustrated. This work provides a clear example of catalytic reaction with explicit structure-activity relationship and highlights the power of zeolite catalysis in complex chemical transformations.
利用可再生氢源将一氧化碳选择性加氢制甲醇是一氧化碳循环利用的一条有吸引力的途径，且具有碳中性。目前正在大力研发具有高活性和甲醇选择性的稳定催化剂，关于活性位点和反应途径的当前争论需要得到澄清。在此，我们报道了一种用于这一具有挑战性反应的八面沸石笼单核铜中心（即Cu@FAU）的设计。在513 K的相对较低反应温度下，同时实现了12.8 mmol g⁻¹ h⁻¹的稳定甲醇时空产率（STY）和89.5%的甲醇选择性，使Cu@FAU成为一种由一氧化碳加氢合成甲醇的潜在催化剂。以沸石笼单核铜中心作为目标活性位点，阐明了在Cu@FAU上一氧化碳逐步加氢的独特反应途径。这项工作提供了一个具有明确结构-活性关系的催化反应的清晰实例，并突出了沸石催化在复杂化学转化中的作用。
