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Continuous CO2 electrolysis using a CO2 exsolution-induced flow cell

Nature Energy volume 7, pages 978–988 (2022)Cite this article

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Abstract

CO2 electrolysis promises a route to carbon-based chemicals and fuels using renewable energy and resources. However, industrial application is limited by the transfer of CO2, electrons, protons and products (CEPP) at high current densities. Here we present an electrolyser that uses the forced convection of an aqueous CO2-saturated catholyte throughout a porous electrode and exploits the in situ formation of CO2(g)–liquid–catalyst interfaces to improve the CEPP transfer and reach high current densities. The CO2 supply is expedited by an increased exsolution of gaseous CO2 from dissolved CO2 and bicarbonate due to the effect of local pressure decreases; simultaneous CEPP transfer is promoted with a tenfold decrease in the diffusion layer thickness. This system also enables catalyst synthesis by in situ electrodeposition and ligand modification. We achieved a maximum current density of 3.37 A cm–2 with a Ag-based catalyst, and assemble a scaled-up 4 × 100 cm2 electrolyser stack that produces CO at a rate of 90.6 l h–1.

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Fig. 1: Concept of flow-through-induced dynamic TPBs.
Fig. 2: Structure and mechanisms of FTDT cell.
Fig. 3: Effects of flow configurations.
Fig. 4: Optimization of FTDT-cell.
Fig. 5: Performance of FTDT cells.
Fig. 6: Performance of the FTDT cell compared with reported data and electrode stability tests.
Fig. 7: The role of bicarbonate in the CO2 supply and transport.
Fig. 8: Extension of proposed FTDT concept to an electrolyser stack and Cu materials for C2+ production.

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Data availability

Source data are provided with this paper. Data generated and analysed in this study are included in the manuscript, Supplementary Information and Supplementary Data.

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Acknowledgements

We acknowledge the support from the University of Waterloo and the Natural Sciences and Engineering Research Council of Canada (NSERC). We gratefully thank the Canadian Light Source and its funding partners. We acknowledge the Vacuum Interconnected Nanotech Workstation (Nano-X) in the Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences (CAS). We acknowledge the financial support provided by the Outstanding Youth Project of the Guangdong Natural Science Foundation (grant no. 2021B1515020051, X.W.), Science and Technology Program of Guangzhou (2019050001, X.W.) and the National 111 Project. This work was also financially supported by the Department of Science and Technology of Guangdong Province (grant no. 2019JC01L203 and no. 2020B0909030004, X.W.) and the Natural Science Foundation of Guangdong Province (no. 2022A1515011804, G.W.). We acknowledge the computational resources from the Shared Hierarchical Academic Research Computing Network (SHARCNET, www.sharcnet.ca), Compute Canada and CMC Microsystems (http://www.cmc.ca).

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  1. These authors contributed equally: Guobin Wen, Bohua Ren.

Authors and Affiliations

  1. Department of Chemical Engineering, Waterloo Institute for Nanotechnology, Waterloo Institute for Sustainable Energy, University of Waterloo, Waterloo, Ontario, Canada

    Guobin Wen, Bohua Ren, Dan Luo, Haozhen Dou, Yun Zheng, Rui Gao, Jeff Gostick, Aiping Yu & Zhongwei Chen

  2. School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangdong, China

    Bohua Ren, Xin Wang & Dan Luo

  3. South China Academy of Advanced Optoelectronics, South China Normal University, Guangdong, China

    Xin Wang

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Contributions

G.W. and Z.C. devised the idea and wrote the manuscript; X.W. and Z.C. supervised the project; G.W. and H.D. synthesized the materials; G.W. and R.G. performed the material and electrode characterizations; A.Y. guided and supervised the characterizations; G.W., B.R., D.L. and Y.Z. performed electrochemical experiments and data analyses; B.R. conducted the density functional theory simulations; G.W. and B.R. designed the cell structures; J.G. supervised the multiphysics simulations; all the authors engaged in the discussion and editing of the manuscript.

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Correspondence to Xin Wang, Aiping Yu or Zhongwei Chen.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–43, Notes 1–21, Methods, Tables 1–9 and references.

Supplementary Video 1

Startup of FTDT-cell for CO2RR.

Supplementary Video 2

FTDT-cell for CO2RR at 2.9 V with a total current of 25 A.

Supplementary Video 3

FTDT-cell for CO2RR at 3.5 V with a total current of 62 A.

Supplementary Video 4

FTDT-cell for CO2RR at 4.0 V with a total current of 90 A with two outlets.

Supplementary Data 1

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Statistical Source Data.

Source Data Fig. 5

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Source Data Fig. 8

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Wen, G., Ren, B., Wang, X. et al. Continuous CO2 electrolysis using a CO2 exsolution-induced flow cell. Nat Energy 7, 978–988 (2022). https://doi.org/10.1038/s41560-022-01130-6

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