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Nano Research 2022, 15(8): 6999-7007 https://doi.org/10.1007/s12274-022-4335-1
Research Article | Issue | Published: 10 May 2022

Industrial-current-density CO2-to-formate conversion with low overpotentials enabled by disorder-engineered metal sites

Show Author's Information Zhiqiang Wang1,§,  Xiaolong Zu1,§,  Xiaodong Li1,§,  Li Li1,  Yang Wu1,  Shumin Wang1,  Peiquan Ling1,  Yuan Zhao1,  Yongfu Sun1,2( ),  Yi Xie1,2
Hefei National Laboratory for Physical Sciences at Microscale, University of Science and Technology of China, Hefei 230026, China
Institute of Energy, Hefei Comprehensive National Science Center, Hefei 230031, China

§ Zhiqiang Wang, Xiaolong Zu, and Xiaodong Li contributed equally to this work.

Keywords:
low overpotential, CO2-to-formate , disorder-engineered, metallic nanosheets, industrial-current-density
Topics:
Catalysis
Cite this article:
Wang Z, Zu X, Li X, et al. Industrial-current-density CO2-to-formate conversion with low overpotentials enabled by disorder-engineered metal sites. Nano Research, 2022, 15(8): 6999-7007. https://doi.org/10.1007/s12274-022-4335-1
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Abstract Full text Electronic supplementary material About this article

CO2 electroreduction to formate is technically feasible and economically viable, but still suffers from low selectivity and high overpotential at industrial current densities. Here, lattice-distorted metallic nanosheets with disorder-engineered metal sites are designed for industrial-current-density CO2-to-formate conversion at low overpotentials. As a prototype, richly lattice-distorted bismuth nanosheets are first constructed, where abundant disorder-engineered Bi sites could be observed by high-angle annular dark-field scanning transmission electron microscopy image. In-situ Fourier-transform infrared spectra reveal the CO2•−* group is the key intermediate, while theoretical calculations suggest the electron-enriched Bi sites could effectively lower the CO2 activation energy barrier by stabilizing the CO2•−* intermediate, further affirmed by the decreased formation energy from 0.49 to 0.39 eV. As a result, the richly lattice-distorted Bi nanosheets exhibit the ultrahigh current density of 800 mA·cm−2 with 91% Faradaic efficiencies for CO2-to-formate electroreduction, and the formate selectivity can reach nearly 100% at the current density of 200 mA·cm−2 with a very low overpotential of ca. 570 mV, outperforming most reported metal-based electrocatalysts.


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About this article

Industrial-current-density CO2-to-formate conversion with low overpotentials enabled by disorder-engineered metal sites

Show Author's information Zhiqiang Wang1,§, Xiaolong Zu1,§, Xiaodong Li1,§, Li Li1, Yang Wu1, Shumin Wang1, Peiquan Ling1, Yuan Zhao1, Yongfu Sun1,2( ), Yi Xie1,2
Hefei National Laboratory for Physical Sciences at Microscale, University of Science and Technology of China, Hefei 230026, China
Institute of Energy, Hefei Comprehensive National Science Center, Hefei 230031, China

§ Zhiqiang Wang, Xiaolong Zu, and Xiaodong Li contributed equally to this work.

Abstract

CO2 electroreduction to formate is technically feasible and economically viable, but still suffers from low selectivity and high overpotential at industrial current densities. Here, lattice-distorted metallic nanosheets with disorder-engineered metal sites are designed for industrial-current-density CO2-to-formate conversion at low overpotentials. As a prototype, richly lattice-distorted bismuth nanosheets are first constructed, where abundant disorder-engineered Bi sites could be observed by high-angle annular dark-field scanning transmission electron microscopy image. In-situ Fourier-transform infrared spectra reveal the CO2•−* group is the key intermediate, while theoretical calculations suggest the electron-enriched Bi sites could effectively lower the CO2 activation energy barrier by stabilizing the CO2•−* intermediate, further affirmed by the decreased formation energy from 0.49 to 0.39 eV. As a result, the richly lattice-distorted Bi nanosheets exhibit the ultrahigh current density of 800 mA·cm−2 with 91% Faradaic efficiencies for CO2-to-formate electroreduction, and the formate selectivity can reach nearly 100% at the current density of 200 mA·cm−2 with a very low overpotential of ca. 570 mV, outperforming most reported metal-based electrocatalysts.

Keywords: low overpotential, CO2-to-formate , disorder-engineered, metallic nanosheets, industrial-current-density

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Publication history
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Acknowledgements

Publication history

Received: 11 January 2022
Revised: 17 February 2022
Accepted: 15 March 2022
Published: 10 May 2022
Issue date: August 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was financially supported by the National Key Research and Development Program of China (No. 2019YFA0210004), the National Natural Science Foundation of China (Nos. 22125503, 21975242, U2032212, and 21890754), the Strategic Priority Research Program of Chinese Academy of Sciences (No. XDB36000000), Youth Innovation Promotion Association of CAS (No. CX2340007003), the Key Research Program of Frontier Sciences of CAS (No. QYZDY-SSW-SLH011), the Major Program of Development Foundation of Hefei Center for Physical Science and Technology (No. 2020HSC-CIP003), Users with Excellence Program of Hefei Science Center CAS (No. 2020HSC-UE001), and the University Synergy Innovation Program of Anhui Province (No. GXXT-2020-001). Supercomputing University of Science and Technology of China (USTC) and the National Supercomputing Center in Shenzhen are acknowledged for computational support.

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