期刊
NATURE COMMUNICATIONS
卷 11, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-020-17738-9
关键词
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资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program
- National Natural Science Foundation of China [21673146, 21802099, 21972098]
- National Key Research & Development Program of China [2016YFC0204901]
- National Engineering Laboratory for Mobile Source Emission Control Technology [NELMS2017A06]
- Sichuan Science and Technology Program [2018GZ0401]
- China Scholarship Council
Single-atom catalysts (SACs) have attracted considerable attention in the catalysis community. However, fabricating intrinsically stable SACs on traditional supports (N-doped carbon, metal oxides, etc.) remains a formidable challenge, especially under high-temperature conditions. Here, we report a novel entropy-driven strategy to stabilize Pd single-atom on the high-entropy fluorite oxides (CeZrHfTiLa)O-x (HEFO) as the support by a combination of mechanical milling with calcination at 900 degrees C. Characterization results reveal that single Pd atoms are incorporated into HEFO (Pd-1@HEFO) sublattice by forming stable Pd-O-M bonds (M=Ce/Zr/La). Compared to the traditional support stabilized catalysts such as Pd@CeO2, Pd-1@HEFO affords the improved reducibility of lattice oxygen and the existence of stable Pd-O-M species, thus exhibiting not only higher low-temperature CO oxidation activity but also outstanding resistance to thermal and hydrothermal degradation. This work therefore exemplifies the superiority of high-entropy materials for the preparation of SACs. Fabricating intrinsically stable single-atom catalysts (SACs) on traditional supports remains a formidable challenge in catalysis. Here, the authors propose a new strategy to construct a sintering-resistant Pd SAC on a novel equimolar high-entropy fluorite oxide.
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