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The structure-dependent catalytic behavior is one of the most important issues in catalysis science. However, it has not been fully understood how different types of atom-packing structures of heterogeneous catalysts precisely impact the reaction sites and pathways. Here we investigate a periodic series of Au8n + 4(TBBT)4n + 8 nanoclusters with layer-by-layer structural pattern to catalyze CO2 hydrogenation (where n = 3-6 is the number of (001) layers; TBBT = 4-tert-butyl-benzenethiolate). An encouraging evolution of CO2 conversion can be identified: The product selectivity from methanol, formic acid to ethanol can be switched by the structure-dependent deformation from the flattened, perfect, to elongated cuboids in Au8n + 4(TBBT)4n + 8. Through a combined study of experiment and theory, we demonstrate that the variation in structural patterns of catalysts can exclusively tune their adsorption strength with reaction intermediates and further control the CO2 conversion toward the different products.

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Publication history
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Acknowledgements

Publication history

Received: 12 July 2020
Revised: 15 August 2020
Accepted: 14 September 2020
Published: 01 March 2021
Issue date: March 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature

Acknowledgements

We acknowledged financial support from the National Natural Science Foundation of China (No. 91961204), the Fundamental Research Funds for the Central Universities, and China Postdoctoral Science Foundation (No. 2019M650106).

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