Abstract
Industrializing the electrosynthesis of formate from CO2 reduction in membrane electrode assembly (MEA) electrolysers necessitates tuning both electrocatalysts and the interfacial water microenvironment. Here we cast a series of Turing-structured topology electrocatalysts, which can control the reorientation of interfacial water through the tuning of surface oxophilicity, for industrial-level conversion of CO2 to formate. Experimental and theoretical results verify the precisely modulated reorientation of interfacial water, with the ratios of four-coordinated to two-coordinated hydrogen-bonded interfacial water ranging from 0.26 to 3.10 over Turing-structured topology catalysts. We further demonstrate the efficiency of these strategies in sustaining high-rate formate electrosynthesis across a wide range of industrial-level current densities (300–1,000 mA cm−2) and formulate a volcano relationship to describe the relation. The optimal Turing Sb0.1Sn0.9O2 catalyst achieves a formate Faradaic efficiency of 92.0% at 1,000 mA cm-2 and exhibits a stability of 200 h at 500 mA cm-2 in a membrane electrode assembly electrolyser. Our findings highlight the prospect of topology-mediated tunings of the interfacial water microenvironment for electrifying the conversion of CO2 to formate, with promising implications for the electrosynthesis of other valuable chemicals.
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Acknowledgements
This work was financially supported by the Science and Technology Innovation Project of Laoshan Laboratory (LSKJ202205400), the National Science Fund for Distinguished Young Scholars (number 52025133), the Beijing Outstanding Young Scientist Program (JWZQ20240102004), the National Science Fund for Young Scholars (numbers 22102003, 22409009), the China National Petroleum Corporation-Peking University Strategic Cooperation Project of Fundamental Research, the Beijing Natural Science Foundation (number Z220020), the Tencent Foundation through the XPLORER PRIZE, the CNPC Innovation Fund (2021DQ02-1002) and the China Postdoctoral Science Foundation (grant number 2023M730052).
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S.G. conceived the project. N.Y. and M.L. designed the research, and performed the material synthesis, characterization and electrochemical tests. K.W., Y.T., Z.Q., Z.L. and Q.H. participated in assembling and testing the MEA. N.Y. and Y.L. carried out the XAFS data analysis. H.G., C.S., Y.H. and C.Z. performed the HAADF-STEM characterization. L.L. and Y.G. conducted the density functional theory calculations. S.G. and N.Y. wrote the paper. All authors participated in the project discussions and production of the final manuscript.
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Nature Synthesis thanks the anonymous reviewers for their contribution to the peer review of this work. Primary Handling Editor: Alexandra Groves, in collaboration with the Nature Synthesis team.
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Ye, N., Wang, K., Tan, Y. et al. Industrial-level CO2 to formate conversion on Turing-structured electrocatalysts. Nat. Synth 4, 799–807 (2025). https://doi.org/10.1038/s44160-025-00769-9
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DOI: https://doi.org/10.1038/s44160-025-00769-9
