Abstract
The development of substrates capable of anchoring single-atom catalysts (SACs) while enabling their dynamic reconfiguration into heteronuclear dual-atom catalysts (DACs) holds considerable promise for electrochemical synthesis, yet remains underexplored. Here we show that electrochemical desulfurization of MoS2 generates vacancy-rich 1T′ domains, which support high loadings of Cu (7.9 wt%) and Pt (6.7 wt%) SACs that are well-positioned for dynamic sintering to form DACs. Operando X-ray absorption spectroscopy and density functional theory calculations reveal a voltage-driven, reversible transformation between individual Pt/Cu SACs and Cu–Pt DAC configurations during hydrogen evolution reaction potentials. The electric-field-induced Cu–Pt DACs exhibit superior performance in the selective hydrogenation of alkynes compared with their monometallic SAC counterparts. This work underscores vacancy-enriched 1T′-MoS2 as a versatile platform for high-density SAC deposition, enabling on-demand structural reconfiguration and paving the way for tailored catalyst design in electrosynthesis.
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Acknowledgements
K.P.L. acknowledges funding support from NUS’s Centre for Hydrogen Innovation program (grant no. CHI-P2022-01). Z.C. acknowledges the University Development Fund, Research Start-up Fund (grant no. UDF01002976). M.Y. acknowledges funding support from the Natural Science Foundation of Guangdong (grant no. P0046476). We acknowledge funding support from the Singapore-International Synchrotron Access Programme (SG-ISAP) and National Synchrotron Programme (NSP). Part of this research was performed on the X-ray absorption spectroscopy beamline at the Australian Synchrotron, which is part of ANSTO; we acknowledge their support for operando XAS experiment. We also thank the National Supercomputing Centre of Singapore for providing computational resources, and the Electron Microscopy Facility (EMF) at National University of Singapore, as well as the Facility for Analysis, Characterisation, Testing and Simulation (FACTS) at Nanyang Technological University, for the STEM measurements. We also thank the staff of the BL17B beamline at the National Facility for Protein Science in Shanghai, Shanghai Advanced Research Institute, Chinese Academy of Sciences, for their technical support in XAFS data collection.
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J.W. conceived the research, synthesized the materials, and performed catalytic measurements under the supervision of K.P.L. X-ray absorption spectroscopy measurements and data processing were performed by J.W. and S.X. Molecular dynamics and DFT calculations were performed by K.Y. under the supervision of M.Y. Scanning transmission electron microscopy characterizations (including electron ptychography/4D-STEM) were performed by X.Z. and M.S. In situ Raman measurements were performed by H.L. under the supervision of C.L. and B.Z. Scanning electron microscopy, partial XAS measurements, STEM data analysis and schematic diagrams were performed by Z.W. R.Z. helped to build the model for the XANES simulation. In situ DRIFTS measurement were performed by T.W. under the supervision of N.Y. Q.H. assisted in testing the XAS. The draft was written by J.W. and revised by K.P.L. All authors discussed and commented on the manuscript.
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Nature Nanotechnology thanks Xin-Hao Li and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Molecular dynamics simulation of the protonation process at the negative voltage
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Wu, J., Chen, Z., Yang, K. et al. Electric bias-induced reversible configuration of single and heteronuclear dual-atom catalysts on 1Tʹ-MoS2. Nat. Nanotechnol. 20, 1043–1051 (2025). https://doi.org/10.1038/s41565-025-01934-z
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DOI: https://doi.org/10.1038/s41565-025-01934-z
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