Journal
SMALL
Volume 16, Issue 38, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202002071
Keywords
crystal facet induced atom trapping; low-temperature catalytic oxidation; metal-support interfaces; Pd single-atom catalysts; tunable cobalt-based nanoarrays
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Funding
- National Natural Science Foundation of China [21736009, 21236008, 21808202]
- Zhejiang Provincial Natural Science Foundation of China [LY18B060010]
- Minjiang Scholarship from Fujian Provincial Government
- Postdoctoral Science Foundation of China [2018M642480]
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Atomic dispersed metal sites in single-atom catalysts are highly mobile and easily sintered to form large particles, which deteriorates the catalytic performance severely. Moreover, lack of criterion concerning the role of the metal-support interface prevents more efficient and wide application. Here, a general strategy is reported to synthesize stable single atom catalysts by crafting on a variety of cobalt-based nanoarrays with precisely controlled architectures and compositions. The highly uniform, well-aligned, and densely packed nanoarrays provide abundant oxygen vacancies (17.48%) for trapping Pd single atoms and lead to the creation of 3D configured catalysts, which exhibit very competitive activity toward low temperature CO oxidation (100% conversion at 90 degrees C) and prominent long-term stability (continuous conversion at 60 degrees C for 118 h). Theoretical calculations show that O vacancies at high-index {112} facet of Co(x)O(y)nanocrystallite are preferential sites for trapping single atoms, which guarantee strong interface adhesion of Pd species to cobalt-based support and play a pivotal role in preventing the decrement of activity, even under moisture-rich conditions (approximate to 2% water vapor). The progress presents a promising opportunity for tailoring catalytic properties consistent with the specific demand on target process, beyond a facile design with a tunable metal-support interface.
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