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Efficient electrocatalytic CO2 reduction on a three-phase interface

Abstract

Electrochemical CO2 reduction is a critical approach to reducing the globally accelerating CO2 emission and generating value-added products. Despite great efforts to optimize catalyst activity and selectivity, facilitating the catalyst accessibility to high CO2 concentrations while maintaining electrode durability remains a significant challenge. Here, we designed a catalytic system that mimics the alveolus structure in mammalian lungs with high gas permeability but very low water diffusibility, enabling an array of three-phase catalytic interfaces. Flexible, hydrophobic, nanoporous polyethylene membranes with high gas permeability were used to enable efficient CO2 access and a high local alkalinity on the catalyst surface at different CO2 flow rates. Such an alveolus-mimicking structure generates a high CO production Faradaic efficiency of 92% and excellent geometric current densities of CO production (25.5 mA cm−2) at −0.6 V versus the reversible hydrogen electrode, with a very thin catalyst thickness of 20−80 nm.

Fig. 1: Schematics of the artificial lung-inspired Au/PE catalyst system for efficient electrocatalytic CO2 reduction.
Fig. 2: Structural characterizations and electrocatalytic CO2 reduction performances of the Au/PE membranes.
Fig. 3: Electrocatalytic performances under different CO2 flow rates.
Fig. 4: Performance comparison of different Au/PE membranes for CO2 and water reduction.

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Acknowledgements

This work was supported by the Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract DEAC02-76-SF00515. The authors acknowledge the use and support of the Stanford Nano Shared Facilities and Stanford Nanofabrication Facility. The authors thank G. Zhou, Z. Lu, W. Chen and L. Cai for helpful discussions. J.L. thanks R. Brinks Lockwood for writing suggestions.

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J.L., S.C. and Y.C. conceived the idea for the project. J.L., Z.L., H.R.L., Y.Z. and H.W. performed the structural characterization. J.L. and Y.Z. performed the theoretical analysis. J.L., G.C, C.-L.W. and K.L. conducted the device fabrication. J.L. conducted the performance measurements and analysed the data. J.L., A.P., S.C. and Y.C. wrote the manuscript. S.C. and Y.C. supervised the project. All authors discussed the results and commented on the manuscript at all stages.

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Correspondence to Yi Cui.

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Supplementary Information

Supplementary Figures 1–22, Supplementary Tables 1–3, Supplementary Notes 1 & 2, Supplementary References

Supplementary Video 1

A movie of bilayer Au/PE membrane under an applied potential of –1.1 V in a CO2-saturated 0.5 M KHCO3 solution containing phenolphthalein. The Au-coated side of PE membrane was rolled to face inside, and the white colour of the pristine PE membrane was facing outwards

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Li, J., Chen, G., Zhu, Y. et al. Efficient electrocatalytic CO2 reduction on a three-phase interface. Nat Catal 1, 592–600 (2018). https://doi.org/10.1038/s41929-018-0108-3

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