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Efficient electrosynthesis of n-propanol from carbon monoxide using a Ag–Ru–Cu catalyst

Nature Energy volume 7, pages 170–176 (2022)Cite this article

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Abstract

The high-energy-density C3 fuel n-propanol is desired from CO2/CO electroreduction, as evidenced by propanol’s high market price per tonne (approximately US$ 1,400–1,600). However, CO electroreduction to n-propanol has shown low selectivity, limited production rates and poor stability. Here we report catalysts, identified using computational screening, that simultaneously facilitate multiple carbon–carbon coupling, stabilize C2 intermediates and promote CO adsorption, all leading to improved n-propanol electrosynthesis. Experimentally we construct the predicted optimal electrocatalyst based on silver–ruthenium co-doped copper. We achieve, at 300 mA cm−2, a high n-propanol Faradaic efficiency of 36% ± 3%, a C2+ Faradaic efficiency of 93% and single-pass CO conversion of 85%. The system exhibits 100 h stable n-propanol electrosynthesis. Technoeconomic analysis based on the performance of the pilot system projects profitability.

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Fig. 1: DFT calculations on C1–C1 and C1–C2 coupling.
Fig. 2: Structural and compositional analyses of the Ag–Ru–Cu catalysts.
Fig. 3: CORR performance of different cathode electrodes.
Fig. 4: In situ characterization and n-propanol electrosynthesis in a larger electrolyser.
Fig. 5: Breakdown of the plant-gate levelized cost per tonne of n-propanol and the corresponding quantity of ethanol, ethylene and H2 produced on Ag–Ru–Cu at a current density of 300 mA cm−2.

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All data are available within the paper, Supplementary Information and source data files. Source data are provided with this paper.

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Acknowledgements

This work was supported by the Natural Sciences and Engineering Research Council (NSERC) of Canada (number RGPIN-2017-06477, E.H.S.) and the Ontario Research Fund—Research Excellence Program (number ORF-RE08-034, E.H.S.). DFT calculations were performed on the Niagara supercomputer at the SciNet HPC Consortium. We acknowledge the computational resources supported by SciNet, which is funded by the University of Toronto, the Ontario Research Fund—Research Excellence Program, the Government of Ontario and the Canada Foundation for Innovation. D.S. acknowledges the NSERC E.W.R. Steacie Memorial Fellowship. Synchrotron measurements were carried out at the BL-17C at the National Synchrotron Radiation Research Center. We thank R. Wolowiec and D. Kopilovic for their kind technical assistance, Ontario Centre for the Characterization of Advanced Materials (OCCAM) of the University of Toronto and the National Synchrotron Radiation Research Center.

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Author notes

  1. F. Pelayo García de Arquer

    Present address: ICFO – Institut de Ciències Fotòniques, Barcelona Institute of Science and Technology, Barcelona, Spain

  2. These authors contributed equally: Xue Wang, Pengfei Ou.

Authors and Affiliations

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

    Xue Wang, Pengfei Ou, Jared Sisler, Koen Bertens, F. Pelayo García de Arquer, Ziyun Wang, Jehad Abed, Armin Sedighian Rasouli, Mengjia Sun, Alexander H. Ip & Edward H. Sargent

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

    Adnan Ozden, Christine M. Gabardo, Rui Kai Miao, Colin P. O’Brien & David Sinton

  3. Department of Applied Chemistry, National Yang Ming Chiao Tung University, Hsinchu, Taiwan

    Sung-Fu Hung

  4. Department of Materials Science and Engineering, University of Toronto, Toronto, Ontario, Canada

    Jason Tam & Jane Y. Howe

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Contributions

E.H.S. supervised the project. X.W. and E.H.S. conceived the idea. X.W. designed and carried out the experiments. P.O. carried out DFT calculations. S.-F.H. performed XAS measurements. S.-F.H. and J.A. analysed the XAS data. A.O. fabricated the IrOx-coated Ti mesh electrodes. J.T. and J.Y.H. contributed to the SEM and TEM characterization. X.W and J.S. did the TEA. K.B. and ASR carried out XPS measurements. X.W. and M.S. performed XRD measurements. C.M.G. and F.P.G.d.A. contributed to the manuscript editing. X.W., P.O., and E.H.S. co-wrote the manuscript. R.K.M., C.P.O, Z.W., A.H.I. and D.S. assisted with the discussions. All authors discussed the results and assisted during manuscript preparation.

Corresponding author

Correspondence to Edward H. Sargent.

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Competing interests

X.W. and E.H.S. have filed a provisional patent application titled ‘Manufacturing and use of co-doped multi-metallic electrocatalysts for upgrading of CO to propanol’ (application number 63/192,842). All other authors declare no competing interests.

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Nature Energy thanks Maximilian Fleischer, Xiaowa Nie and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Wang, X., Ou, P., Ozden, A. et al. Efficient electrosynthesis of n-propanol from carbon monoxide using a Ag–Ru–Cu catalyst. Nat Energy 7, 170–176 (2022). https://doi.org/10.1038/s41560-021-00967-7

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