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Highly active and stable stepped Cu surface for enhanced electrochemical CO2 reduction to C2H4

Nature Catalysis volume 3, pages 804–812 (2020)Cite this article

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Abstract

Electrochemical CO2 reduction to value-added chemical feedstocks is of considerable interest for renewable energy storage and renewable source generation while mitigating CO2 emissions from human activity. Copper represents an effective catalyst in reducing CO2 to hydrocarbons or oxygenates, but it is often plagued by a low product selectivity and limited long-term stability. Here we report that copper nanowires with rich surface steps exhibit a remarkably high Faradaic efficiency for C2H4 that can be maintained for over 200 hours. Computational studies reveal that these steps are thermodynamically favoured compared with Cu(100) surface under the operating conditions and the stepped surface favours C2 products by suppressing the C1 pathway and hydrogen production.

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Fig. 1: Schematic of preparing CuNWs with surface steps.
Fig. 2: TEM characterizations of the Syn-CuNW and A-CuNW.
Fig. 3: Electrochemical characterization of the surfaces of the CuNWs.
Fig. 4: Electrochemical CO2RR performance.
Fig. 5: The stability and activity of the Cu(511) step surface.

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The data that support the findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

The TEM work was conducted using the facilities in the Electron Imaging Center at the California NanoSystems Institute at the University of California Los Angles and the Irvine Materials Research Institute at the University of California Irvine. C.C., J.C., X.D. and Y.H. acknowledge support from the Office of Naval Research (ONR) under grant no. N000141712608. S.K., T.C. and W.A.G. were supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under Award no. DE-SC0004993. C.L., S.K. and H.M.L. used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant no. ACI-1548562. C.L. and H.M.L. were also supported by a National Research Foundation (NRF) of Korea grant funded by the Korean Government (no. NRF-2017R1E1A1A03071049). The work done at the University of California Irvine was supported by the Irvine Materials Research Institute and ExxonMobil.

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Authors and Affiliations

  1. Department of Materials Science and Engineering, University of California, Los Angeles, Los Angeles, CA, USA

    Chungseok Choi, Changsoo Lee, Jin Cai & Yu Huang

  2. Department of Applied Physics and Materials Science, California Institute of Technology, Pasadena, CA, USA

    Soonho Kwon, Tao Cheng & William A. Goddard III

  3. Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, P. R. China

    Tao Cheng

  4. Irvine Materials Research Institute (IMRI), University of California, Irvine, Irvine, CA, USA

    Mingjie Xu & Xiaoqing Pan

  5. Department of Materials Science and Engineering, University of California, Irvine, Irvine, CA, USA

    Mingjie Xu & Xiaoqing Pan

  6. Fok Ying Tung Research Institute, The Hong Kong University of Science and Technology, Guangzhou, P. R. China

    Mingjie Xu

  7. Department of Chemistry, University of California, Irvine, Irvine, CA, USA

    Peter Tieu

  8. Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, Yuseong-gu, Republic of Korea

    Changsoo Lee & Hyuck Mo Lee

  9. Department of Physics and Astronomy, University of California, Irvine, Irvine, CA, USA

    Xiaoqing Pan

  10. Department of Chemistry and Biochemistry, University of California, Los Angeles, Los Angeles, CA, USA

    Xiangfeng Duan

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  1. Chungseok Choi
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Contributions

C.C. designed and conducted most of the experiments, analysed all the data and prepared the manuscript. S.K., T.C. and W.A.G. performed the density theoretical calculations and prepared the manuscript. M.X., P.T. and X.P. took SEI and bright-field scanning transmission electron microscopy images. J.C., C.L., H.M.L and X.D. assisted in the experiments and the preparation of the manuscript. Y.H. initiated the study, oversaw the project and wrote the manuscript. All the authors discussed the results and contributed to the manuscript.

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Correspondence to William A. Goddard III or Yu Huang.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–15, Tables 1–6 and references.

Supplementary Data 1

Atomic structures of the initial state, transition state and final state

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Choi, C., Kwon, S., Cheng, T. et al. Highly active and stable stepped Cu surface for enhanced electrochemical CO2 reduction to C2H4. Nat Catal 3, 804–812 (2020). https://doi.org/10.1038/s41929-020-00504-x

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