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

Public Time: 2020-08-06 00:00:00
Journal: Nature Communications
doi: 10.1038/s41467-020-17738-9
Author: Haidi Xu;Zihao Zhang;Jixing Liu;Chi-Linh Do-Thanh;Hao Chen;Shuhao Xu;Qinjing Lin;Yi Jiao;Jianli Wang;Yun Wang;Yaoqiang Chen;Sheng Dai
Summary: 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.
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