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Synergetic interaction between neighbouring platinum monomers in CO2 hydrogenation

Abstract

Exploring the interaction between two neighbouring monomers has great potential to significantly raise the performance and deepen the mechanistic understanding of heterogeneous catalysis. Herein, we demonstrate that the synergetic interaction between neighbouring Pt monomers on MoS2 greatly enhanced the CO2 hydrogenation catalytic activity and reduced the activation energy relative to isolated monomers. Neighbouring Pt monomers were achieved by increasing the Pt mass loading up to 7.5% while maintaining the atomic dispersion of Pt. Mechanistic studies reveal that neighbouring Pt monomers not only worked in synergy to vary the reaction barrier, but also underwent distinct reaction paths compared with isolated monomers. Isolated Pt monomers favour the conversion of CO2 into methanol without the formation of formic acid, whereas CO2 is hydrogenated stepwise into formic acid and methanol for neighbouring Pt monomers. The discovery of the synergetic interaction between neighbouring monomers may create a new path for manipulating catalytic properties.

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Fig. 1: Structural characterizations of Pt/MoS2.
Fig. 2: Catalytic performance of Pt/MoS2 in the hydrogenation of CO2.
Fig. 3: The interaction between reactants and Pt/MoS2.
Fig. 4: DFT studies.

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Acknowledgements

This work was supported by Collaborative Innovation Center of Suzhou Nano Science and Technology, Ministry of Science and Technology of the People’s Republic of China (2014CB932700 and 2016YFA0200602), National Natural Science Foundation of China (21573206 and 21473167), Key Research Program of Frontier Sciences of the Chinese Academy of Sciences (QYZDB-SSW-SLH017), Anhui Provincial Key Scientific and Technological Project (1704a0902013), Anhui Provincial Natural Science Foundation (1608085QB29), Major Program of Development Foundation of Hefei Center for Physical Science and Technology (2017FXZY002), Fundamental Research Funds for the Central Universities, Shanghai Supercomputing Center and Supercomputing Center at the University of Science and Technology of China.

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H.L., L.W. and J.Zeng designed the studies and wrote the paper. H.L., L.W., Y.D. and Z.P. synthesized the catalysts. H.L., L.W., Y.C., Z.L. and M.W. performed catalytic tests. C.M. conducted HAADF-STEM analysis. H.L. and W.Z. performed DFT calculations. L.W., X.Z. and J.Zhu conducted XPS measurements. R.S. conducted XAFS measurements. All authors discussed the results and commented on the manuscript.

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Correspondence to Wenhua Zhang or Jie Zeng.

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Li, H., Wang, L., Dai, Y. et al. Synergetic interaction between neighbouring platinum monomers in CO2 hydrogenation. Nature Nanotech 13, 411–417 (2018). https://doi.org/10.1038/s41565-018-0089-z

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