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Research Article

The role of CO2 dissociation in CO2 hydrogenation to ethanol on CoCu/silica catalysts

Zhongyan Wang1, Chengsheng Yang1, Xianghong Li1, Xiwen Song1, Chunlei Pei1, Zhi-Jian Zhao1( ), Jinlong Gong1,2,3
Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin University, Tianjin 300072, China
Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, China
Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China
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Abstract

CoCu-based catalysts are widely used in COx hydrogenation reactions to produce higher alcohols due to the C–C coupling ability of Co and the ability of Cu to produce alcohols. This work describes the role of easily happened CO2 dissociation on the CoCu surface during the reaction, using different silica support to tune the metal–support interaction, and reaches different selectivity to ethanol. CoCu supported on mesoporous silica MCM-41 shows ethanol selectivity as high as 85.3%, and the ethanol space-time yield (STY) is 0.229 mmol/(gmetal∙h), however, poor selectivity to ethanol as low as 28.8% is observed on CoCu supported on amorphous silica. The different selectivity is due to the different intensities of CO2 dissociation on the catalysts. The adsorbed O* produced via CO2 dissociation can occupy the cobalt hollow sites on CoCu surfaces, which are also the adsorption sites of C1 intermediates for further C–C coupling.

Graphical Abstract

CO2 can dissociate on CoCu catalysts supported on different silica supports. The interaction between metal nanoparticles and support can infect the C–C dissociation process, tuning the intermediate adsorbed on active sites. CoCu/MCM-41 catalysts can dissociate CO2 moderately, leaving sufficient active sites for C–C coupling and selectivity of C2+ products. On the other hand, CO2 dissociates rapidly on CoCu/SiO2, resulting in active sites occupied, inhibiting C–C coupling.

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Nano Research
Pages 6128-6133

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Cite this article:
Wang Z, Yang C, Li X, et al. The role of CO2 dissociation in CO2 hydrogenation to ethanol on CoCu/silica catalysts. Nano Research, 2023, 16(5): 6128-6133. https://doi.org/10.1007/s12274-022-5092-x
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Received: 06 May 2022
Revised: 14 September 2022
Accepted: 24 September 2022
Published: 18 November 2022
© Tsinghua University Press 2022