Abstract
Dual-atom catalysts (DACs) exhibit high catalytic activity and metal utilization, alongside structural diversity with a wide range of catalytic site configurations. These features position DACs as promising candidates for energy conversion technologies. However, the precise control over atomic dispersion, pairing ratios and interatomic distances—which critically influence their multifunctional catalytic behavior—remains a formidable challenge. Here we developed a ligand-restricted strategy for the precise synthesis of highly paired DACs with tunable atomic distances. This was accomplished by coordinating diamine ligands with dual-metal precursors, restricting the pairing and relative positions of two metal atoms on two-dimensional graphitic carbon nitride. The atomic pairing ratio exceeded 82%, and the atomic pairing distance was controlled by the chain length of the diamine ligand. As a demonstration, the paired Pt1-Au1 DACs exhibited almost threefold enhancement in catalytic activity for nitrate reduction to ammonia compared with their unpaired counterparts. This work introduces an effective strategy for the atomic-scale fabrication of complex catalysts as well as provides valuable insights into nanoscale reaction mechanisms in heterogeneous catalysis.
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Acknowledgements
This research was financially supported by the National Key Research and Development Program of China (2022YFA1205200 to L.W.), the National Natural Science Foundation of China (52033003 to L.W., 22279139 to J.L., 62227815 to J.L., 22202027 to S.L. and 22572012 to S.L.), Program of Higher-Level Talents of IMU (10000-23112101/173 to J.L.), Project of Grassland Talent of Inner Mongolia Autonomous Region (12000-12102805 to J.L.) and the Natural Science Foundation of Inner Mongolia Autonomous Region of China (20241Q06 to J.L.). We thank C. Li, R. Che, J. Liang, P.-C. Chen, H. Tan, Y. Gu, W. Tu, J. Du and Y. Hao for helpful discussion.
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This study was conceived by J.L. and L.W. Y.M. carried out the synthesis, characterization and catalytic measurements. S.L. and W. Liu contributed to the electron-microscopy-based atom recognition statistics methodology. W.Z., R.Z., K.S. and R.G. performed the DFT calculations and analysis. W. Li carried out the catalytic performance. J.M. and Z.J. performed the XAS measurement and analysed the data. Y.M., Y.Z., S.L., J.S. and W. Liu performed the AC-HAADF-STEM characterization. M.S. and B.H. performed the DFT and ML. Y.M., G.Q.M.L., J.L. and L.W. wrote the paper. All authors were involved in discussions on the paper.
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Ma, Y., Liu, S., Mao, J. et al. Ligand-restricted synthesis of highly paired dual-atom catalysts. Nat. Mater. 25, 80–90 (2026). https://doi.org/10.1038/s41563-025-02385-6
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DOI: https://doi.org/10.1038/s41563-025-02385-6
