Journal
ACS CATALYSIS
Volume 9, Issue 4, Pages 3144-3152Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b04741
Keywords
high-index facets; model catalysts; single crystalline planes; electrocatalysis; electrooxidation; structure-reactivity relationship
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Funding
- National Key Research and Development Program of China [2017YFA0206500]
- Natural Science Foundation of China [21573181, 21603103, 91645121, 21621091]
- UK EPSRC [EP/I013229/1]
- Natural Science Foundation Committee of Jiangsu Province [BK20171462]
- EPSRC [EP/I013229/1] Funding Source: UKRI
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Knowledge of the structure-reactivity relationship of catalysts is usually gained through using well-defined bulk single-crystal planes as model catalysts. However, there exists a huge gap between bulk single-crystal planes and practical nanocatalysts in terms of size, structural complexity, and local environment. Herein, we efficiently bridged this gap by developing a model nanocatalyst based on nanocrystals with continuously tunable surface structures. Pd nanocrystals with finely tunable facets, ranging from a flat {100} low-index facet to a series of {hk0} high-index facets, were prepared by an electrochemical square-wave potential method. The validity of the Pd model nanocatalyst has been demonstrated by structure-reactivity studies of electrocatalytic oxidation of small organic molecules. We further observed that Pd nanocrystals exhibited catalytic performance considerably different from bulk Pd single-crystal planes with the same Miller indices. Such differences were attributed to special catalytic functions conferred by nanocrystal edges. This study paves a promising route for investigating catalytic reactions effectively at the atomic level and nanoscales.
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