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Cationic-group-functionalized electrocatalysts enable stable acidic CO2 electrolysis

Nature Catalysis volume 6, pages 763–772 (2023)Cite this article

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Abstract

Acidic electrochemical CO2 reduction (CO2R) addresses CO2 loss and thus mitigates the energy penalties associated with CO2 recovery; however, acidic CO2R suffers low selectivity. One promising remedy—using a high concentration of alkali cations—steers CO2R towards multi-carbon (C2+) products, but these same alkali cations result in salt formation, limiting operating stability to <15 h. Here we present a copper catalyst functionalized with cationic groups (CG) that enables efficient CO2 activation in a stable manner. By replacing alkali cations with immobilized benzimidazolium CG within ionomer coatings, we achieve over 150 h of stable CO2R in acid. We find the water-management property of CG minimizes proton migration that enables operation at a modest voltage of 3.3 V with mildly alkaline local pH, leading to more energy-efficient CO2R with a C2+ Faradaic efficiency of 80 ± 3%. As a result, we report an energy efficiency of 28% for acidic CO2R towards C2+ products and a single-pass CO2 conversion efficiency exceeding 70%.

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Fig. 1: Computational studies of CG-functionalized catalysts in acidic CO2R.
Fig. 2: Cationic functional group enables CO2R in acidic media.
Fig. 3: Performance of the CG-functionalized catalysts in acid media.
Fig. 4: Stability and SPC performance of carbon-protected CG-medium Cu in acidic media.

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Data availability

Source data for the stability test shown in Fig. 4a,b and the atomic coordinates of the optimized computational models can be found in figshare26. Data that support the findings of this study can be found in the article and Supplementary information. All other data supporting this work are available from the corresponding authors upon reasonable request.

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Acknowledgements

We acknowledge support from the Natural Sciences and Engineering Research Council (NSERC) of Canada and TotalEnergies SE. Support from Canada Research Chairs Program is also gratefully acknowledged. Infrastructure provided through the Canada Foundation for Innovation and the Ontario Research Fund supported the work. R.K.M. thanks NSERC, Hatch and the Government of Ontario for their support through graduate scholarships. P.O. thanks the Climate Positive Energy for its support through Rising Stars in Clean Energy Postdoctoral Fellowship. Density functional theory calculations were performed on the Niagara supercomputer at the SciNet HPC Consortium. SciNet is funded by: the Canada Foundation for Innovation; the Government of Ontario; Ontario Research Fund - Research Excellence; and the University of Toronto. The computational study is supported by the Marsden Fund Council from Government funding (21-UOA-237) and Catalyst: Seeding General Grant (22-UOA-031-CGS), managed by Royal Society Te Apārangi. Z.W. and Y.M. acknowledge the use of New Zealand eScience Infrastructure (NeSI) high-performance computing facilities, consulting support and/or training services as part of this research. G.I.N.W. and Y.M. acknowledge funding support from the MacDiarmid Institute for Advanced Materials and Nanotechnology, the Energy Education Trust of New Zealand and the Royal Society Te Apārangi. Z.W. and Y.M. graciously acknowledge D. J. Searles (University of Queensland) and J. Cheng (Xiamen University) for their support and scientific discussions on the computational work.

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Author notes

  1. These authors contributed equally: Mengyang Fan, Jianan Erick Huang, Rui Kai Miao, Yu Mao, Pengfei Ou.

Authors and Affiliations

  1. Department of Mechanical and Industrial Engineering, University of Toronto, Toronto, Ontario, Canada

    Mengyang Fan, Rui Kai Miao, Feng Li, Jinqiang Zhang, Adnan Ozden, Yong Zhao, Behrooz Khatir, Colin P. O’Brien, Yi Xu, Yurou Celine Xiao, Kevin Golovin & David Sinton

  2. Department of Electrical and Computer Engineering, University of Toronto, Toronto, Ontario, Canada

    Jianan Erick Huang, Pengfei Ou, Xiao-Yan Li, Yufei Cao, Jinqiang Zhang, Yu Yan, Weiyan Ni, Zhu Chen & Edward H. Sargent

  3. School of Chemical Sciences, The University of Auckland, Auckland, New Zealand

    Yu Mao, Geoffrey I. N. Waterhouse & Ziyun Wang

  4. Department of Chemistry, Northwestern University, Evanston, IL, USA

    Pengfei Ou & Edward H. Sargent

  5. Department of Chemistry, The University of British Columbia, Vancouver, British Columbia, Canada

    Zishuai Zhang

  6. Department of Chemistry, The Chinese University of Hong Kong S. A. R., Ma Liu Shui, China

    Ying Wang

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  1. Mengyang Fan
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Contributions

D.S. and E.H.S. supervised the project. M.F., J.E.H. and R.K.M. designed and carried out all the experiments. J.E.H. conceived the idea. Y.M., P.O. and Y.C. carried out the MD simulation. Z.W. supervised the MD simulation. Y.M., Y.C., G.I.N.W. and Z.W. analysed the MD simulation results. M.F. and J.E.H. analysed the experimental data and prepared the paper. R.K.M. performed the slim-flow cell design and experiments. F.L. carried out the COMSOL simulation. M.F. carried out all EIS measurements and analysed data. J.E.H. and Z.C. carried out the SERS measurements, and M.F. analysed the SERS data. Z.Z. performed the pH-sensitive Raman tests. J.Z., A.O. and Y.W. synthesized catalysts. W.N. and Y.Z. carried out scanning electron microscopy characterization. Y.Y. performed the X-ray diffraction characterization. B.K. and K.G. carried out the contact angle measurements. C.P.O., Y.X. and Y.C.X. performed product analysis. All authors discussed the results and assisted during paper preparation.

Corresponding authors

Correspondence to Ziyun Wang, Edward H. Sargent or David Sinton.

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Competing interests

There is a US provisional patent application (63/381.180) titled ‘A modified catalyst for operating electrochemical carbon dioxide reduction in a non-alkali acidic medium and related techniques’, filed by the authors M.F., J.E.H., R.K.M., E.H.S. and D.S of this article and their institutions. The other authors declare no competing interests.

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Fan, M., Huang, J.E., Miao, R.K. et al. Cationic-group-functionalized electrocatalysts enable stable acidic CO2 electrolysis. Nat Catal 6, 763–772 (2023). https://doi.org/10.1038/s41929-023-01003-5

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