Abstract
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)Ox (HEFO) as the support by a combination of mechanical milling with calcination at 900 °C. Characterization results reveal that single Pd atoms are incorporated into HEFO (Pd1@HEFO) sublattice by forming stable Pd–O–M bonds (M = Ce/Zr/La). Compared to the traditional support stabilized catalysts such as Pd@CeO2, Pd1@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.
Original language | English |
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Article number | 3908 |
Journal | Nature Communications |
Volume | 11 |
Issue number | 1 |
DOIs | |
State | Published - Dec 1 2020 |
Funding
Z.Z., J.L., C.D., H.C., and S.D. were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. H.X., S.X., Q.L., Y.J., and Y.W. were supported by the National Natural Science Foundation of China (Nos. 21802099, 21972098), National Key Research & Development Program of China (No. 2016YFC0204901), National Engineering Laboratory for Mobile Source Emission Control Technology (No. NELMS2017A06) and Sichuan Science and Technology Program (No. 2018GZ0401). Y.C. and J.W. were supported by the National Natural Science Foundation of China (No. 21673146). H.X. also thanks the China Scholarship Council for financial support as a visiting scholar. Authors thank Dr. Miaomiao Liu in East China University of Science and Technology for giving the comments on the Scheme and Ms. Jia Li in Sichuan University for the models of HEFO and Pd1@HEFO. Ceshigo Research Service for agency STEM and XAS, www.ceshigo.com.