Laser Ablation and Fragmentation in Liquid Synthesis of Novel Palladium-Sulfur Compound Nanoparticles as Efficient Electrocatalysts for Hydrogen Evolution Reaction

Abstract One promising way to tune the physicochemical properties of materials and optimize their performance in various potential applications is to engineer material structures at the atomic level. As well known, the performance of Pd-based catalysts has long been constrained by surface contamination and their single structure. Here, we employed an unadulterated top-down laser ablation synthesis method, known as laser fragmentation in liquid (LFL), to modify pristine PdPS crystals and obtained a kind of metastable palladium sulfur compound nanoparticles (LFL-PdS NPs) as a highly efficient electrocatalyst for hydrogen evolution reaction (HER). Laser fragmentation of the layered PdPS crystal led to a structural reorganization at the atomic level and resulted in the formation of uniform metastable LFL-PdS NPs. Noteworthy, the LFL-PdS NPs show excellent electrocatalytic HER performance and stability in acidic media, with an overpotential of -66 mV at 10 mA cm-2, the Tafel slope of 42 mV dec-1. The combined catalytic performances of our LFL-PdS NPs are fully comparable to the Pt/C catalyst for HER. This work provided a top-down synthesis strategy as a promising approach to design highly active metastable metal composite electrocatalysts for sustainable energy applications.