Abstract

Metal particles supported on oxide surfaces are used as catalysts for a wide variety of processes in the chemical and energy conversion industries. For catalytic applications, metal particles are generally formed on an oxide support by physical or chemical deposition, or less commonly by exsolution from it. Although fundamentally different, both methods might be assumed to produce morphologically and functionally similar particles. Here we show that unlike nickel particles deposited on perovskite oxides, exsolved analogues are socketed into the parent perovskite, leading to enhanced stability and a significant decrease in the propensity for hydrocarbon coking, indicative of a stronger metal–oxide interface. In addition, we reveal key surface effects and defect interactions critical for future design of exsolution-based perovskite materials for catalytic and other functionalities. This study provides a new dimension for tailoring particle–substrate interactions in the context of increasing interest for emergent interfacial phenomena.

Highlights

  • Metal particles supported on oxide surfaces are used as catalysts for a wide variety of processes in the chemical and energy conversion industries

  • Previous studies demonstrated that catalytically active transition metals can be substituted on the B-site of perovskite oxides (ABO3), in oxidizing conditions, and released on the surface as metal particles following reduction (Supplementary Fig. 1b), with applications in catalysis ranging from automotive emission control to solid oxide fuel/electrolysis cells[11,12,13,14,15,16,17]

  • We employ compositions derived from SrTiO3, an archetype oxide of considerable interest for applications ranging from solid oxide fuel cells to complex oxide electronics[19,20,21,22]

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Summary

Introduction

Metal particles supported on oxide surfaces are used as catalysts for a wide variety of processes in the chemical and energy conversion industries. The vast majority of supported particles are prepared by deposition methods (for example, infiltration, Supplementary Fig. 1a), which widely applicable, provide limited control over particle interaction with the support, during deposition and over time[4,5]. This leads to deactivation by agglomeration[5] or by coking (carbon accumulation on the metal in hydrocarbon environment) in industrially critical processes such as syngas production by methane steam reforming[6,7]. We provide critical insights into surface effects and defect interactions relevant for the future development of exsolution process and for perovskite bulk or surface related applications

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