Abstract
Electrochemical hydrogenation of quinoxaline presents a promising alternative to traditional methods, yet is suffering from low current density and Faradaic efficiency due to the hampered hydrogenation process. Herein, we develop a cocatalytic system of Ru single atoms doped Co3O4 nanosheet (RuSA/ns-Co3O4) to optimize the interfacial H2O behavior by tuning the Ru single atoms concentration for accelerating the electrochemical hydrogenation of quinoxaline, which enables remarkable Faradaic efficiency of 82% toward 1,2,3,4-tetrahydroquinoxaline at high current density of 200 mA cm-2. Detailed experimental and theoretical studies reveal that Ru single atoms trigger interfacial charge redistribution, inducing an asymmetric local electric field that reconstructs interfacial H2O molecules into an H-down configuration. This reorientation remodels the hydrogen-bonded water network, shortens the distance between hydrogen atoms and the Co3O4 surface, regulates K•H2O availability, and enhances H2O dissociation to supply H*. Consequently, the membrane electrode assembly electrolyser exhibits a long-term stability of >100 h at 200 mA cm-2. Our findings highlight the prospect of interfacial water microenvironment for electrochemical hydrogenation of unsaturated N-heterocyclic compounds, with promising applications for the electrosynthesis of other valuable chemicals.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (no. 52371221 and U23A20554 to Y.W.T.) and Independent Research Project of State Key Laboratory of Advanced Design and Manufacturing Technology for Vehicle Body (no. 72365004 to Y.W.T.). The Raman and STEM tests were performed at the Analytical Instrumentation Center of Hunan University. In situ XAS tests were performed at Shanghai Synchrotron Radiation Facility (SSRF).
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Y.W.T. conceived and directed the project. L.H.M. carried out key experiments. T.Y.D., T.H.W., and Q.J. performed theoretical calculations. J.L.L. contributed to the XAS measurements and analyses of the XAS experiment results. C.J.D., F.Y.W., and M.P. contributed to the data analysis. Y.W.T. and L.H.M. wrote the manuscript with input from all other authors. All authors discussed the results and commented on the manuscript.
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Nature Communications thanks Xiao Chen, Kai Liu, Lingxia Zheng and the other anonymous reviewer(s) for their contribution to the peer review of this work. A peer review file is available.
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Meng, L., Dai, Ty., Li, J. et al. Interfacial water regulation on Ru single atoms doped Co3O4 toward efficient electrochemical hydrogenation of quinoxaline. Nat Commun (2026). https://doi.org/10.1038/s41467-026-68740-6
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DOI: https://doi.org/10.1038/s41467-026-68740-6
