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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, Sheng Dai

2020Nature Communications386 citationsDOIOpen Access PDF

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)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.

Topics & Concepts

FluoriteCatalysisCalcinationOxideMaterials scienceHydrothermal circulationMetalAtom (system on chip)Transition metalChemical engineeringCrystallographyChemistryMetallurgyOrganic chemistryComputer scienceEngineeringEmbedded systemCatalytic Processes in Materials ScienceHigh Entropy Alloys StudiesCatalysis and Oxidation Reactions