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

• Published in: Nature communications Vol. 11; no. 1; p. 3908
• Main Authors: Xu, Haidi, Zhang, Zihao, Liu, Jixing, Do-Thanh, Chi-Linh, Chen, Hao, Xu, Shuhao, Lin, Qinjing, Jiao, Yi, Wang, Jianli, Wang, Yun, Chen, Yaoqiang, Dai, Sheng
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 06-08-2020; Nature Publishing Group; Nature Portfolio
• Subjects: 140/146; 147/143; 639/638/77/884; 639/638/77/887; 639/638/898; Catalysis; Catalysts; Cerium oxides; Entropy; Fluorite; High temperature; Humanities and Social Sciences; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Low temperature; Mechanical milling; Metal oxides; multidisciplinary; Oxidation; Oxidation resistance; Oxides; Palladium; PD-1 protein; Science; Science (multidisciplinary); Single atom catalysts; Thermal resistance; Zirconium
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-020-17738-9

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 °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@CeO
2
, 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.