Entropy-stabilized single-atom Pd catalysts via high-entropy fluorite oxide supports

Haidi Xu, Zihao Zhang, Jixing Liu, Chi-Linh Do-Thanh, Hao Chen, Shuhao Xu, Qinjing Lin, Yi Jiao, Jianli Wang, Yun Wang (), Yaoqiang Chen () and Sheng Dai ()
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Haidi Xu: Sichuan University
Zihao Zhang: Chemical Sciences Division, Oak Ridge National Laboratory
Jixing Liu: University of Tennessee
Chi-Linh Do-Thanh: University of Tennessee
Hao Chen: University of Tennessee
Shuhao Xu: Sichuan University
Qinjing Lin: Sichuan University
Yi Jiao: Sichuan University
Jianli Wang: Sichuan University
Yun Wang: Sinocat Environmental Technology Co. Ltd.
Yaoqiang Chen: Sichuan University
Sheng Dai: Chemical Sciences Division, Oak Ridge National Laboratory

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-17738-9

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