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Regulating socketed geometry of nanoparticles on perovskite oxide supports for enhanced stability in oxidation reactions

Jihang YuState Key Laboratory of Green Chemical Engineering and Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, PR ChinaXinwei YangState Key Laboratory of Green Chemical Engineering and Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, PR ChinaYanyan JiaKey Laboratory for Advanced Materials, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, PR ChinaZhi-Qiang WangState Key Laboratory of Green Chemical Engineering and Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, PR ChinaWenbo LiKey Laboratory for Advanced Materials, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, PR ChinaYongjun JiangKey Laboratory for Advanced Materials, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, PR ChinaSheng DaiKey Laboratory for Advanced Materials, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, PR China. [email protected]Wangcheng ZhanState Key Laboratory of Green Chemical Engineering and Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, PR China. [email protected]

2024en

ABI

Annotatsiya

Heterogeneous catalysts with highly dispersed active particles on supports often face stability challenges during high-temperature industrial applications. The ex-solution strategy, which involves in situ extrusion of metals to form socketed particles, shows potential for addressing this stability issue. However, a deeper understanding of the relationship between the socketed geometry of these partially embedded nanoparticles and their catalytic performance is still lacking. Here, in situ transmission electron microscopy and theoretical calculations are utilized to investigate the oxygen-induced ex-solution process of Pd-doped LaAlO3 with varying concentrations of La vacancies (LaxAl0.9Pd0.1O3-δ). We find that the socketed geometry of Pd-based particles can be tuned by manipulating the levels of La deficiencies in the oxide support, which in turn influences the catalytic performance in high-temperature oxidation reactions. As for the socketed particles, the balance between particle size and outcrop height is crucial for determining the oxidation activity and sinter-resistance behavior. Consequently, the optimized catalyst, La0.8Al0.9Pd0.1O3-δ, exhibits superior catalytic performances, particularly high stability (still working after aging at 1000 °C for 50 h) and water resistance in various combustion reactions (e.g., CH4 oxidation and C3H8 oxidation). Nanoparticles with precisely controlled socketed geometries, created via an ex-solution method, present promising ways to improve the stability of heterogeneous catalysts. Here, the authors demonstrate that adjusting the level of La deficiencies in the oxide support allows tuning of the geometry of Pd-based particles, which in turn influences their catalytic performance in high-temperature oxidation reactions.

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DOI: 10.1038/s41467-024-54546-x

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