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Electrocatalytic dual hydrogenation of organic substrates with a Faradaic efficiency approaching 200%

Nature Catalysis volume 6, pages 224–233 (2023)Cite this article

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Abstract

The wide deployment of electrocatalytic hydrogenation may be hindered by intrinsic limitations, including substrate solubility and difficult separation of the products from the electrolyte. The use of palladium membrane electrodes can overcome the aforementioned limitations by physically separating the formation of reactive hydrogen atoms from the hydrogenation of unsaturated organic substrates. Here, by taking advantage of the low-potential oxidation of formaldehyde on a palladium membrane anode to produce hydrogen that can permeate through the membrane electrode, we demonstrate that electrocatalytic dual hydrogenation of unsaturated dicarboxylic acids is possible when another palladium membrane electrode is also adopted as the cathode. Such a design enables the electrocatalytic hydrogenation of the same substrate at both the anode and cathode in two separated chambers spatially isolated from the electrochemical cell with a theoretical maximum Faradaic efficiency of 200%.

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Fig. 1: Schematics of three different electrocatalytic hydrogenation designs.
Fig. 2: Comparison of electrocatalytic H2 production and absorption using Pd electrodes.
Fig. 3: Electrocatalytic dual hydrogenation of maleic acid.
Fig. 4: Electrocatalytic dual hydrogenation under various conditions.
Fig. 5: Versatility of electrocatalytic dual hydrogenation.
Fig. 6: Investigation of the hydrogen source.

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The data that support the findings of this study are included in the published article and the Supplementary Information. Further queries about the data can be directed to the corresponding author. Source data are provided with this paper.

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Acknowledgements

Y.S. acknowledges the financial support of the National Science Foundation (CHE-1914546 and CHE-2102220), the Herman Frasch Foundation (820-HF17), the Michelman Green, Clean and Sustainable Technology Research Innovation Program, and the University of Cincinnati.

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Authors and Affiliations

  1. Department of Chemistry, University of Cincinnati, Cincinnati, OH, USA

    Guanqun Han, Guodong Li & Yujie Sun

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  1. Guanqun Han
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Contributions

Y.S. conceived the idea and supervised the project. G.H. and G.L. performed the experimental work and data analysis. G.H. and Y.S. wrote the manuscript.

Corresponding author

Correspondence to Yujie Sun.

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Competing interests

Y.S. has filed a provisional patent application related to this manuscript (US patent provisional 63/440,044). All other authors declare no competing interests.

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Nature Catalysis thanks Shuangyin Wang, Hongyuan Sheng and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Methods, Figs. 1–45 and ref. 1.

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Han, G., Li, G. & Sun, Y. Electrocatalytic dual hydrogenation of organic substrates with a Faradaic efficiency approaching 200%. Nat Catal 6, 224–233 (2023). https://doi.org/10.1038/s41929-023-00923-6

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