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Enhancing acetate selectivity by coupling anodic oxidation to carbon monoxide electroreduction

Nature Catalysis volume 5, pages 738–745 (2022)Cite this article

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Abstract

Electrocatalytic conversion of carbon monoxide (CO) is being actively developed as a key component for tandem CO2 electrolysis. Great effort has been devoted to engineering CO reduction electrocatalysts for better multicarbon product selectivity. However, less work has focused on other performance parameters that are crucial for commercializing CO electrolysis, such as liquid product concentration and purity. Here, we present an internally coupled purification strategy to substantially improve the acetate concentration and purity in CO electrolysis. This strategy utilizes an alkaline-stable anion exchange membrane with high ethanol permeability and a selective ethanol partial oxidation anode to control the CO reduction product stream. We demonstrate stable 120-h continuous operation of the CO electrolyser at a current density of 200 mA cm−2 and a full-cell potential of <2.3 V, continuously producing a 1.9 M acetate product stream with a purity of 97.7%. The acetate stream was further improved to a concentration of 7.6 M at >99% purity by tuning the reaction conditions. Finally, a techno-economic analysis shows that a highly concentrated liquid product stream is essential to reduce the energy consumption of product separation.

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Fig. 1: Production of concentrated acetate streams via eCOR.
Fig. 2: Anodic impact on selectivity via the partial oxidation of alcohols.
Fig. 3: Membrane crossover rate influence on eCOR selectivity.
Fig. 4: Techno-economic assessment of recirculative acetate production.

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Data availability

All data is available from the authors upon reasonable request. Source data are provided with this paper.

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Acknowledgements

This material is based upon work supported by the US Department of Energy under Award Number DE-FE0031910.

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Authors and Affiliations

  1. Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, USA

    Sean Overa, Bradie S. Crandall, Byung Hee Ko, Haeun Shin & Feng Jiao

  2. Department of Chemistry and Chemical Biology, Rensselaer Polytechnic Institute, Troy, NY, USA

    Bharat Shrimant, Ding Tian & Chulsung Bae

  3. The Howard P. Isermann Department of Chemical and Biological Engineering, Rensselaer Polytechnic Institute, Troy, NY, USA

    Chulsung Bae

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  1. Sean Overa
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Contributions

S.O. conducted the experiments, performed the data analysis and wrote the first draft of the manuscript. B.S.C. conducted the techno-economic analysis. B.S. and D.T. produced and conducted the analysis of the anion exchange membrane. B.H.K. performed the XPS measurements and analysed the XPS data. H.S. conducted the scanning electron microscopy measurements. C.B. supervised the synthesis of the anion exchange membranes. F.J. revised the manuscript and supervised the whole project. All authors commented on the final version of the manuscript.

Corresponding author

Correspondence to Feng Jiao.

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Supplementary Information

Supplementary Notes 1–5, Figs. 1–43 and Tables 1–8.

Source data

Source Data Fig. 1

Data for 120-h durability in Fig. 1b.

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Overa, S., Crandall, B.S., Shrimant, B. et al. Enhancing acetate selectivity by coupling anodic oxidation to carbon monoxide electroreduction. Nat Catal 5, 738–745 (2022). https://doi.org/10.1038/s41929-022-00828-w

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