Surface passivation for highly active, selective, stable, and scalable CO2 electroreduction

Jiexin Zhu; Jiantao Li; Ruihu Lu; Ruohan Yu; Shiyong Zhao; Chengbo Li; Lei Lv; Lixue Xia; Xingbao Chen; Wenwei Cai; Jiashen Meng; Wei Zhang; Xuelei Pan; Xufeng Hong; Yuhang Dai; Yu Mao; Jiong Li; Liang Zhou; Guanjie He; Quanquan Pang; Yan Zhao; Chuan Xia; Ziyun Wang; Liming Dai; Liqiang Mai

doi:10.1038/s41467-023-40342-6

Surface passivation for highly active, selective, stable, and scalable CO₂ electroreduction

Jiexin Zhu, Jiantao Li, Ruihu Lu, Ruohan Yu, Shiyong Zhao, Chengbo Li, Lei Lv, Lixue Xia, Xingbao Chen, Wenwei Cai, Jiashen Meng, Wei Zhang, Xuelei Pan, Xufeng Hong, Yuhang Dai, Yu Mao, Jiong Li, Liang Zhou, Guanjie He, Quanquan PangYan Zhao, Chuan Xia^*, Ziyun Wang^*, Liming Dai^*, Liqiang Mai^*

^*Corresponding author for this work

Chemical and Biological Engineering

Research output: Contribution to journal › Article › peer-review

73 Scopus citations

Abstract

Electrochemical conversion of CO₂ to formic acid using Bismuth catalysts is one the most promising pathways for industrialization. However, it is still difficult to achieve high formic acid production at wide voltage intervals and industrial current densities because the Bi catalysts are often poisoned by oxygenated species. Herein, we report a Bi₃S₂ nanowire-ascorbic acid hybrid catalyst that simultaneously improves formic acid selectivity, activity, and stability at high applied voltages. Specifically, a more than 95% faraday efficiency was achieved for the formate formation over a wide potential range above 1.0 V and at ampere-level current densities. The observed excellent catalytic performance was attributable to a unique reconstruction mechanism to form more defective sites while the ascorbic acid layer further stabilized the defective sites by trapping the poisoning hydroxyl groups. When used in an all-solid-state reactor system, the newly developed catalyst achieved efficient production of pure formic acid over 120 hours at 50 mA cm^–2 (200 mA cell current).

Original language	English (US)
Article number	4670
Journal	Nature communications
Volume	14
Issue number	1
DOIs	https://doi.org/10.1038/s41467-023-40342-6
State	Published - Dec 2023

Funding

L.M. acknowledges the National Key Research and Development Program of China (2020YFA0715000), National Natural Science Foundation of China (51832004, 52127816), National Energy-Saving and Low-Carbon Materials Production and Application Demonstration Platform Program (TC220H06N). J.Z. acknowledges the Fundamental Research Funds for the Central Universities (195101005, 2020III004GX). L.D. acknowledges the Australian Research Council (FL 190100126, CE230100032). We thank the Beamline 12-BM-B at the Advanced Photon Source and Beamline BL11B at the Shanghai Synchrotron Radiation Facility for XAFS measurement. This S/TEM work was performed at the Nanostructure Research Center (NRC), which is supported by the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, and the State Key Laboratory of Silicate Materials for Architectures. The computational study is supported by the Marsden Fund Council from Government funding, managed by the Royal Society Te Apārangi. Z.W. and R.L. acknowledge the use of New Zealand eScience Infrastructure (NeSI) high performance computing facilities, consulting support and/or training services as part of this research. New Zealand’s national facilities are provided by NeSI and funded jointly by NeSI’s collaborator institutions and through the Ministry of Business, Innovation & Employment’s Research Infrastructure programme. URL https://www.nesi.org.nz . L.M. acknowledges the National Key Research and Development Program of China (2020YFA0715000), National Natural Science Foundation of China (51832004, 52127816), National Energy-Saving and Low-Carbon Materials Production and Application Demonstration Platform Program (TC220H06N). J.Z. acknowledges the Fundamental Research Funds for the Central Universities (195101005, 2020III004GX). L.D. acknowledges the Australian Research Council (FL 190100126, CE230100032). We thank the Beamline 12-BM-B at the Advanced Photon Source and Beamline BL11B at the Shanghai Synchrotron Radiation Facility for XAFS measurement. This S/TEM work was performed at the Nanostructure Research Center (NRC), which is supported by the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, and the State Key Laboratory of Silicate Materials for Architectures. The computational study is supported by the Marsden Fund Council from Government funding, managed by the Royal Society Te Apārangi. Z.W. and R.L. acknowledge the use of New Zealand eScience Infrastructure (NeSI) high performance computing facilities, consulting support and/or training services as part of this research. New Zealand’s national facilities are provided by NeSI and funded jointly by NeSI’s collaborator institutions and through the Ministry of Business, Innovation & Employment’s Research Infrastructure programme. URL https://www.nesi.org.nz.

ASJC Scopus subject areas

General Chemistry
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy

Access to Document

10.1038/s41467-023-40342-6

Cite this

Zhu, J., Li, J., Lu, R., Yu, R., Zhao, S., Li, C., Lv, L., Xia, L., Chen, X., Cai, W., Meng, J., Zhang, W., Pan, X., Hong, X., Dai, Y., Mao, Y., Li, J., Zhou, L., He, G., ... Mai, L. (2023). Surface passivation for highly active, selective, stable, and scalable CO₂ electroreduction. Nature communications, 14(1), Article 4670. https://doi.org/10.1038/s41467-023-40342-6

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abstract = "Electrochemical conversion of CO2 to formic acid using Bismuth catalysts is one the most promising pathways for industrialization. However, it is still difficult to achieve high formic acid production at wide voltage intervals and industrial current densities because the Bi catalysts are often poisoned by oxygenated species. Herein, we report a Bi3S2 nanowire-ascorbic acid hybrid catalyst that simultaneously improves formic acid selectivity, activity, and stability at high applied voltages. Specifically, a more than 95% faraday efficiency was achieved for the formate formation over a wide potential range above 1.0 V and at ampere-level current densities. The observed excellent catalytic performance was attributable to a unique reconstruction mechanism to form more defective sites while the ascorbic acid layer further stabilized the defective sites by trapping the poisoning hydroxyl groups. When used in an all-solid-state reactor system, the newly developed catalyst achieved efficient production of pure formic acid over 120 hours at 50 mA cm–2 (200 mA cell current).",

author = "Jiexin Zhu and Jiantao Li and Ruihu Lu and Ruohan Yu and Shiyong Zhao and Chengbo Li and Lei Lv and Lixue Xia and Xingbao Chen and Wenwei Cai and Jiashen Meng and Wei Zhang and Xuelei Pan and Xufeng Hong and Yuhang Dai and Yu Mao and Jiong Li and Liang Zhou and Guanjie He and Quanquan Pang and Yan Zhao and Chuan Xia and Ziyun Wang and Liming Dai and Liqiang Mai",

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Zhu, J, Li, J, Lu, R, Yu, R, Zhao, S, Li, C, Lv, L, Xia, L, Chen, X, Cai, W, Meng, J, Zhang, W, Pan, X, Hong, X, Dai, Y, Mao, Y, Li, J, Zhou, L, He, G, Pang, Q, Zhao, Y, Xia, C, Wang, Z, Dai, L & Mai, L 2023, 'Surface passivation for highly active, selective, stable, and scalable CO₂ electroreduction', Nature communications, vol. 14, no. 1, 4670. https://doi.org/10.1038/s41467-023-40342-6

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AU - Li, Jiantao

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AU - Li, Chengbo

AU - Lv, Lei

AU - Xia, Lixue

AU - Chen, Xingbao

AU - Cai, Wenwei

AU - Meng, Jiashen

AU - Zhang, Wei

AU - Pan, Xuelei

AU - Hong, Xufeng

AU - Dai, Yuhang

AU - Mao, Yu

AU - Li, Jiong

AU - Zhou, Liang

AU - He, Guanjie

AU - Pang, Quanquan

AU - Zhao, Yan

AU - Xia, Chuan

AU - Wang, Ziyun

AU - Dai, Liming

AU - Mai, Liqiang

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