Lowering C−C coupling barriers for efficient electrochemical CO2 reduction to C2H4 by jointly engineering single Bi atoms and oxygen vacancies on CuO

Wenjie Li; Lifen Li; Qineng Xia; Song Hong; Lijun Wang; Zhibo Yao; Tai Sing Wu; Yun Liang Soo; Hao Zhang; Tsz Woon Benedict Lo; Alex W. Robertson; Qingya Liu; Leiduan Hao; Zhenyu Sun

doi:10.1016/j.apcatb.2022.121823

Lowering C−C coupling barriers for efficient electrochemical CO₂ reduction to C₂H₄ by jointly engineering single Bi atoms and oxygen vacancies on CuO

Wenjie Li, Lifen Li, Qineng Xia, Song Hong, Lijun Wang, Zhibo Yao, Tai Sing Wu, Yun Liang Soo, Hao Zhang, Tsz Woon Benedict Lo, Alex W. Robertson, Qingya Liu, Leiduan Hao, Zhenyu Sun

The Hong Kong Polytechnic University

Research output: Journal article publication › Journal article › Academic research › peer-review

46 Citations (Scopus)

Abstract

Electrochemical CO₂ reduction (ECR) to commodity chemicals offers a promising way for mitigating the greenhouse effect and driving the transition from fossil-fuel dependence to a sustainable economy. To this end, the design and development of active and robust electrocatalysts is key. Here we report for the first time that incorporation of bismuth (Bi) single atoms on defective CuO could significantly enhance the ECR reaction to C₂H₄ by decreasing C–C coupling barriers. The overpotential for C₂H₄ production is lowered by at least 50 mV, along with a two-fold improvement in the faradaic efficiency, reaching 60% at 400 mA cm⁻². The high performance is maintained even after 20 h of consecutive electrolysis. Control experiments along with density functional theory calculations suggest that the joint incorporation of Bi and oxygen vacancies greatly promotes CO₂ adsorption and lowers C–C coupling energy barriers, thereby improving the C₂H₄ selectivity.

Original language	English
Article number	121823
Journal	Applied Catalysis B: Environmental
Volume	318
DOIs	https://doi.org/10.1016/j.apcatb.2022.121823
Publication status	Published - 5 Dec 2022

Keywords

Bismuth single atom
CO reduction
Electrolysis
Ethylene
Oxygen vacancy

ASJC Scopus subject areas

Catalysis
General Environmental Science
Process Chemistry and Technology

More information

10.1016/j.apcatb.2022.121823

Cite this

Li, W., Li, L., Xia, Q., Hong, S., Wang, L., Yao, Z., Wu, T. S., Soo, Y. L., Zhang, H., Lo, T. W. B., Robertson, A. W., Liu, Q., Hao, L., & Sun, Z. (2022). Lowering C−C coupling barriers for efficient electrochemical CO₂ reduction to C₂H₄ by jointly engineering single Bi atoms and oxygen vacancies on CuO. Applied Catalysis B: Environmental, 318, Article 121823. https://doi.org/10.1016/j.apcatb.2022.121823

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title = "Lowering C−C coupling barriers for efficient electrochemical CO2 reduction to C2H4 by jointly engineering single Bi atoms and oxygen vacancies on CuO",

abstract = "Electrochemical CO2 reduction (ECR) to commodity chemicals offers a promising way for mitigating the greenhouse effect and driving the transition from fossil-fuel dependence to a sustainable economy. To this end, the design and development of active and robust electrocatalysts is key. Here we report for the first time that incorporation of bismuth (Bi) single atoms on defective CuO could significantly enhance the ECR reaction to C2H4 by decreasing C–C coupling barriers. The overpotential for C2H4 production is lowered by at least 50 mV, along with a two-fold improvement in the faradaic efficiency, reaching 60% at 400 mA cm−2. The high performance is maintained even after 20 h of consecutive electrolysis. Control experiments along with density functional theory calculations suggest that the joint incorporation of Bi and oxygen vacancies greatly promotes CO2 adsorption and lowers C–C coupling energy barriers, thereby improving the C2H4 selectivity.",

keywords = "Bismuth single atom, CO reduction, Electrolysis, Ethylene, Oxygen vacancy",

author = "Wenjie Li and Lifen Li and Qineng Xia and Song Hong and Lijun Wang and Zhibo Yao and Wu, {Tai Sing} and Soo, {Yun Liang} and Hao Zhang and Lo, {Tsz Woon Benedict} and Robertson, {Alex W.} and Qingya Liu and Leiduan Hao and Zhenyu Sun",

note = "Funding Information: This work was supported by the National Natural Science Foundation of China (No. 21972010 ), Beijing Natural Science Foundation (No. 2192039 ), and Fundamental Research Funds for the Central Universities ( buctrc12060096098 ). Publisher Copyright: {\textcopyright} 2022 Elsevier B.V.",

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month = dec,

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doi = "10.1016/j.apcatb.2022.121823",

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journal = "Applied Catalysis B: Environmental",

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Li, W, Li, L, Xia, Q, Hong, S, Wang, L, Yao, Z, Wu, TS, Soo, YL, Zhang, H, Lo, TWB, Robertson, AW, Liu, Q, Hao, L & Sun, Z 2022, 'Lowering C−C coupling barriers for efficient electrochemical CO₂ reduction to C₂H₄ by jointly engineering single Bi atoms and oxygen vacancies on CuO', Applied Catalysis B: Environmental, vol. 318, 121823. https://doi.org/10.1016/j.apcatb.2022.121823

TY - JOUR

T1 - Lowering C−C coupling barriers for efficient electrochemical CO2 reduction to C2H4 by jointly engineering single Bi atoms and oxygen vacancies on CuO

AU - Li, Wenjie

AU - Li, Lifen

AU - Xia, Qineng

AU - Hong, Song

AU - Wang, Lijun

AU - Yao, Zhibo

AU - Wu, Tai Sing

AU - Soo, Yun Liang

AU - Zhang, Hao

AU - Lo, Tsz Woon Benedict

AU - Robertson, Alex W.

AU - Liu, Qingya

AU - Hao, Leiduan

AU - Sun, Zhenyu

N1 - Funding Information: This work was supported by the National Natural Science Foundation of China (No. 21972010 ), Beijing Natural Science Foundation (No. 2192039 ), and Fundamental Research Funds for the Central Universities ( buctrc12060096098 ). Publisher Copyright: © 2022 Elsevier B.V.

PY - 2022/12/5

Y1 - 2022/12/5

N2 - Electrochemical CO2 reduction (ECR) to commodity chemicals offers a promising way for mitigating the greenhouse effect and driving the transition from fossil-fuel dependence to a sustainable economy. To this end, the design and development of active and robust electrocatalysts is key. Here we report for the first time that incorporation of bismuth (Bi) single atoms on defective CuO could significantly enhance the ECR reaction to C2H4 by decreasing C–C coupling barriers. The overpotential for C2H4 production is lowered by at least 50 mV, along with a two-fold improvement in the faradaic efficiency, reaching 60% at 400 mA cm−2. The high performance is maintained even after 20 h of consecutive electrolysis. Control experiments along with density functional theory calculations suggest that the joint incorporation of Bi and oxygen vacancies greatly promotes CO2 adsorption and lowers C–C coupling energy barriers, thereby improving the C2H4 selectivity.

AB - Electrochemical CO2 reduction (ECR) to commodity chemicals offers a promising way for mitigating the greenhouse effect and driving the transition from fossil-fuel dependence to a sustainable economy. To this end, the design and development of active and robust electrocatalysts is key. Here we report for the first time that incorporation of bismuth (Bi) single atoms on defective CuO could significantly enhance the ECR reaction to C2H4 by decreasing C–C coupling barriers. The overpotential for C2H4 production is lowered by at least 50 mV, along with a two-fold improvement in the faradaic efficiency, reaching 60% at 400 mA cm−2. The high performance is maintained even after 20 h of consecutive electrolysis. Control experiments along with density functional theory calculations suggest that the joint incorporation of Bi and oxygen vacancies greatly promotes CO2 adsorption and lowers C–C coupling energy barriers, thereby improving the C2H4 selectivity.

KW - Bismuth single atom

KW - CO reduction

KW - Electrolysis

KW - Ethylene

KW - Oxygen vacancy

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