Pt-modulated Cu/SiO2 catalysts for efficient hydrogenation of CO2-derived ethylene carbonate to methanol and ethylene glycol

doi:10.1016/j.cjche.2021.10.024

Chinese Journal of Chemical Engineering ›› 2022, Vol. 41 ›› Issue (1): 366-373.DOI: 10.1016/j.cjche.2021.10.024

• Catalysis, Kinetics and Reaction Engineering • Previous Articles Next Articles

Pt-modulated Cu/SiO₂ catalysts for efficient hydrogenation of CO₂-derived ethylene carbonate to methanol and ethylene glycol

Busha Assaba Fayisa¹, Yushan Xi¹, Youwei Yang¹, Yueqi Gao¹, Antai Li¹, Mei-Yan Wang^1,2,3, Jing Lv^1,2, Shouying Huang^1,2,3, Yue Wang^1,2,3, Xinbin Ma^1,2,3

1 Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2 Zhejiang Institute of Tianjin University, Ningbo 315201, China;
3 Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, China

Received:2021-08-06 Revised:2021-10-14 Online:2022-02-25 Published:2022-01-28
Contact: Jing Lv,E-mail address:muddylj@tju.edu.cn;Yue Wang,E-mail address:yuewang@tju.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (22022811, U21B2096 and 21938008), the National Key Research & Development Program of China (2018YFB0605803).

Pt-modulated Cu/SiO₂ catalysts for efficient hydrogenation of CO₂-derived ethylene carbonate to methanol and ethylene glycol

Busha Assaba Fayisa¹, Yushan Xi¹, Youwei Yang¹, Yueqi Gao¹, Antai Li¹, Mei-Yan Wang^1,2,3, Jing Lv^1,2, Shouying Huang^1,2,3, Yue Wang^1,2,3, Xinbin Ma^1,2,3

1 Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2 Zhejiang Institute of Tianjin University, Ningbo 315201, China;
3 Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, China

通讯作者: Jing Lv,E-mail address:muddylj@tju.edu.cn;Yue Wang,E-mail address:yuewang@tju.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (22022811, U21B2096 and 21938008), the National Key Research & Development Program of China (2018YFB0605803).

Abstract

Abstract: Copper-based catalysts were widely used in the heterogeneous selective hydrogenation of ethylene carbonate (EC), a key step in the indirect conversion of CO₂ to methanol. However, a high H₂/EC molar ratio in feed is required to achieve favorable activity and the methanol selectivity still needs to be improved. Herein, we fabricated a series of Pt-modulated Cu/SiO₂ catalysts and investigated their catalytic performance for hydrogenation of EC in a fixed bed reactor. By modulating the Pt amount, the optimal 0.2PtCu/SiO₂ catalyst exhibited the highest catalytic performance with ~99% EC conversion, over 98% selectivity to ethylene glycol and 95.8% selectivity to methanol at the H₂/EC ratio as low as 60 in feed. In addition, 0.2Pt-Cu/SiO₂ catalyst showed excellent stability for 150 h on stream over different H₂/EC ratios of 180-40. It is demonstrated a proper amount of Pt could significantly lower the H₂/EC molar ratio, promote the reducibility and dispersion of copper, and also enhance surface density of Cu⁺ species. This could be due to the strong interaction of Cu and Pt induced by formation of alloyed Pt single atoms on the Cu lattice. Meanwhile, a relatively higher amount of Pt would deteriorate the catalytic activity, which could be due to the surface coverage and aggregation of active species. These findings may enlighten some fundamental insights for further design of Cu-based catalysts for the hydrogenation of carbon–oxygen bonds.

Key words: CO₂, Ethylene carbonate, Hydrogenation, Pt-Cu/SiO₂ catalyst, Ethylene glycol, Methanol

摘要： Copper-based catalysts were widely used in the heterogeneous selective hydrogenation of ethylene carbonate (EC), a key step in the indirect conversion of CO₂ to methanol. However, a high H₂/EC molar ratio in feed is required to achieve favorable activity and the methanol selectivity still needs to be improved. Herein, we fabricated a series of Pt-modulated Cu/SiO₂ catalysts and investigated their catalytic performance for hydrogenation of EC in a fixed bed reactor. By modulating the Pt amount, the optimal 0.2PtCu/SiO₂ catalyst exhibited the highest catalytic performance with ~99% EC conversion, over 98% selectivity to ethylene glycol and 95.8% selectivity to methanol at the H₂/EC ratio as low as 60 in feed. In addition, 0.2Pt-Cu/SiO₂ catalyst showed excellent stability for 150 h on stream over different H₂/EC ratios of 180-40. It is demonstrated a proper amount of Pt could significantly lower the H₂/EC molar ratio, promote the reducibility and dispersion of copper, and also enhance surface density of Cu⁺ species. This could be due to the strong interaction of Cu and Pt induced by formation of alloyed Pt single atoms on the Cu lattice. Meanwhile, a relatively higher amount of Pt would deteriorate the catalytic activity, which could be due to the surface coverage and aggregation of active species. These findings may enlighten some fundamental insights for further design of Cu-based catalysts for the hydrogenation of carbon–oxygen bonds.

关键词: CO₂, Ethylene carbonate, Hydrogenation, Pt-Cu/SiO₂ catalyst, Ethylene glycol, Methanol

Busha Assaba Fayisa, Yushan Xi, Youwei Yang, Yueqi Gao, Antai Li, Mei-Yan Wang, Jing Lv, Shouying Huang, Yue Wang, Xinbin Ma. Pt-modulated Cu/SiO₂ catalysts for efficient hydrogenation of CO₂-derived ethylene carbonate to methanol and ethylene glycol[J]. Chinese Journal of Chemical Engineering, 2022, 41(1): 366-373.

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Pt-modulated Cu/SiO₂ catalysts for efficient hydrogenation of CO₂-derived ethylene carbonate to methanol and ethylene glycol

Pt-modulated Cu/SiO₂ catalysts for efficient hydrogenation of CO₂-derived ethylene carbonate to methanol and ethylene glycol

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