Pd Thickness Optimization on Silicate Sheets for Improving Catalytic Activity

Abstract

Abstract Maximizing surface‐to‐body ratio demands ever smaller metallic palladium (Pd) nanoparticles for catalytic applications. The quest for miniaturization is now reaching the single‐atom limit. However, if the supported Pd is below a critical size, the Pd hybridization with the supporting material can detrimentally reduce the labile electrons that facilitate the catalytic reactions. Thus, the smallest attainable size, i.e., single‐atom Pd, may not offer the best efficiency. Here, it is demonstrated that Pd with at least six atomic layers (or thickness of ≈1 nm) on the silicate sheets, synthesized via the partial exfoliation of a layered silicate, exhibits a metallic‐like electronic property, yielding an excellent catalytic activity (e.g., turnover frequency) for dehydrogenating formic acid higher than both isotropic Pd nanoparticles and single‐atom Pd.

Keywords

• density functional theory
• electronic localization function
• H 2 production
• layered silicate
• palladium nanoparticle