Zeolite-encaged mononuclear copper centers catalyze CO2 selective hydrogenation to methanol

Author:

Chai Yuchao1,Qin Bin1,Li Bonan2,Dai Weili3,Wu Guangjun1,Guan Naijia3,Li Landong13ORCID

Affiliation:

1. Key Laboratory of Advanced Energy Materials Chemistry of Ministry of Education, College of Chemistry, Nankai University , Tianjin 300071, China

2. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023, China

3. School of Materials Science and Engineering, Nankai University , Tianjin 300350, China

Abstract

ABSTRACT The selective hydrogenation of CO2 to methanol by renewable hydrogen source represents an attractive route for CO2 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 gcat-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 CO2 hydrogenation. With zeolite-encaged mononuclear Cu centers as the destined active sites, the unique reaction pathway of stepwise CO2 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.

Funder

National Natural Science Foundation of China

China National Postdoctoral Program for Innovative Talents

Fundamental Research Funds for the Central Universities

Publisher

Oxford University Press (OUP)

Subject

Multidisciplinary

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