Zeolite-encaged mononuclear copper centers catalyze CO_(2)selective hydrogenation to methanol  

作　　者：Yuchao Chai Bin Qin Bonan Li Weili Dai Guangjun Wu Naijia Guan Landong Li 

机构地区：[1]Key Laboratory of Advanced Energy MaterialsChemistry of Ministry of Education,Collegeof Chemistry,Nankai University,Tianjin 300071,China [2]Schoolof Materials Scienceand Engineering,Nankai University,Tianjin 300350,China [3]CASKeyLaboratory of Scienceand Technology on Applied Catalysis,Dalian Instituteof Chemical Physics,Chinese Academyof Sciences,Dalian116023,China

出　　处：《National Science Review》2023年第7期129-136,共8页国家科学评论（英文版）

基　　金：supported by the National Natural Science Foundation of China(22121005,22002062 and 22025203);the China National Postdoctoral Program for Innovative Talents(BX20200171);the Fundamental Research Funds for the Central Universities(Nankai University)。

摘　　要：The selective hydrogenation of CO_(2) to methanol by renewable hydrogen source represents an attractive route for CO_(2) 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_(cat)^(-1)h^(-1)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_(2) hydrogenation.With zeolite-encaged mononuclear Cu centers as the destined active sites,the unique reaction pathway of stepwise CO_(2)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.

关 键 词：CO_(2)hydrogenation ZEOLITE METHANOL catalysis mononuclear copper 

分 类 号：TQ426[化学工程] TQ223.121