Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 22, Pages 6464-6469Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201800925
Keywords
density functional calculations; heterogeneous catalysis; supported nanoparticles; surface chemistry; transmission electron microscopy
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Funding
- National Natural Science Foundation of China [11404230, 11604357, 21773287, 11574340, 51390474, 91645103]
- Foundation of Science and Technology Bureau of Sichuan Province [2013JY0085]
- Ministry of Science and Technology of China [2016YFE0105700]
- Natural Science Foundation of Shanghai [16ZR1443200]
- Youth Innovation Promotion Association of Chinese Academy of Sciences
- Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund [U1501501]
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Metal nanoparticles (NPs) dispersed on a high surface-area support are normally used as heterogeneous catalysts. Recent in situ experiments have shown that structure reconstruction of the NP occurs in real catalysis. However; the role played by supports in these processes is still unclear. Supports can be very important in real catalysis because of the new active sites at the perimeter interface between nano particles and supports. Herein, using a developed multiscale model coupled with in situ spherical aberration corrected (Cs-corrected) TEM experiments; we show that the interaction between the support and the gas environment greatly changes the contact surface between the metal and support, which further leads to the critical change in the perimeter interface. The dynamic changes chcnzges of the interface in reactive environments can thus be predicted and be included in the rational design of Supported metal nanocatalysts. In particular, our multiscale model shows quantitative consistency with experimental observations This work offers possibilities for obtaining atomic scale structures and insights beyond the experimental limits.
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