Journal
NATURE CATALYSIS
Volume 3, Issue 10, Pages 834-842Publisher
NATURE RESEARCH
DOI: 10.1038/s41929-020-00511-y
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Funding
- European Research Council program [741431-2DNanoSpec]
- Natural Science Foundation of China [21925404, 21775127, 21703181]
- Fundamental Research Funds for the Central Universities [20720190044]
- MOST [2019YFA0705402]
- Chinese Scholarship Council
- Sino-Swiss Science and Technology Cooperation program [EG22-122016]
- Swiss National Science Foundation [175696]
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Understanding the mechanism of catalytic hydrogenation at the local environment requires chemical and topographic information involving catalytic sites, active hydrogen species, and their spatial distribution. Here we used tip-enhanced Raman spectroscopy (TERS) to study the catalytic hydrogenation of chloronitrobenzenethiol on a well-defined Pd(submonolayer)/Au(111) bimetallic catalyst (pH(2) = 1.5 bar, 298 K), where the surface topography and chemical fingerprint information were simultaneously mapped with nanoscale resolution (similar to 10 nm). TERS imaging of the surface after catalytic hydrogenation confirms that the reaction occurs beyond the location of Pd sites. The results demonstrate that hydrogen spillover accelerates hydrogenation at Au sites as far as 20 nm from the bimetallic Pd/Au boundary. Density functional theory was used to elucidate the thermodynamics of interfacial hydrogen transfers. We demonstrate TERS to be a powerful analytical tool that provides a unique approach to spatially investigate the local structure-reactivity relationship in catalysis.
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