Atomically dispersed metal catalysts maximize atom efficiency and display unique catalytic properties compared with regular metal nanoparticles. However, achieving high reactivity while preserving high stability at appreciable loadings remains challenging. Here we solve the challenge by synergizing metal–support interactions and spatial confinement, which enables the fabrication of highly loaded atomic nickel (3.1 wt%) along with dense atomic copper grippers (8.1 wt%) on a graphitic carbon nitride support. For the semi-hydrogenation of acetylene in excess ethylene, the fabricated catalyst shows extraordinary catalytic performance in terms of activity, selectivity and stability—far superior to supported atomic nickel alone in the absence of a synergizing effect. Comprehensive characterization and theoretical calculations reveal that the active nickel site confined in two stable hydroxylated copper grippers dynamically changes by breaking the interfacial nickel–support bonds on reactant adsorption and making these bonds on product desorption. Such a dynamic effect confers high catalytic performance, providing an avenue to rationally design efficient, stable and highly loaded, yet atomically dispersed, catalysts.
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This work was supported by the National Key R&D Program of China (2018YFA0208603 and 2017YFA0402800); the National Natural Science Foundation of China (22025205, 21673215, 91645202, 91845203, 11621063 and 91945302); the Frontier Science Key Project of the Chinese Academy of Sciences (CAS) (QYZDJ-SSW-SLH054); the Dalian National Laboratory for Clean Energy (DNL) Cooperation Fund (DNL201907 and DNL201920); Beijing Outstanding Young Scientist Program (BJJWZYJH01201914430039); Key Research Program of Frontier Sciences, CAS (QYZDB-SSW-JSC019); Bureau of Frontier of Sciences and Education, CAS (ZDBS-LY-SLH003); the Fundamental Research Funds for the Central Universities (WK2060030029 and WK3430000005); Users with Excellence Program of Hefei Science Center, CAS (2019HSC-UE016); and the Max Planck Partner Group. We also gratefully thank the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF), and the BL10B and BL04B beamlines at the National Synchrotron Radiation Laboratory (NSRL), China, and the Supercomputing Center, University of Science and Technology of China.
The authors declare no competing interests.
Peer review information Nature Nanotechnology thanks Dehui Deng and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Gu, J., Jian, M., Huang, L. et al. Synergizing metal–support interactions and spatial confinement boosts dynamics of atomic nickel for hydrogenations. Nat. Nanotechnol. 16, 1141–1149 (2021). https://doi.org/10.1038/s41565-021-00951-y