High-Yield Electrochemical Production of Large-Sized and Thinly Layered NiPS3 Flakes for Overall Water Splitting

Abstract

Achieving large‐sized and thinly layered 2D metal phosphorus trichalcogenides with high quality and yield has been an urgent quest due to extraordinary physical/chemical characteristics for multiple applications. Nevertheless, current preparation methodologies suffer from uncontrolled thicknesses, uneven morphologies and area distributions, long processing times, and inferior quality. Here, a sonication‐free and fast (in minutes) electrochemical cathodic exfoliation approach is reported that can prepare large‐sized (typically ≈150 µm2) and thinly layered (≈70% monolayer) NiPS3 flakes with high crystallinity and pure phase structure with a yield ≈80%. During the electrochemical exfoliation process, the tetra‐n‐butylammonium salt with a large ionic diameter is decomposed into gaseous species after the intercalation and efficiently expands the tightly stratified bulk NiPS3 crystals, as revealed by in situ and ex situ characterizations. Atomically thin NiPS3 flakes can be obtained by slight manual shaking rather than sonication, which largely preserves in‐plane structural integrity with large size and minimum damage. The obtained high quality NiPS3 offers a new and ideal model for overall water splitting due to its inherent fully exposed S and P atoms that are often the active sites for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Consequently, the bifunctional NiPS3 exhibits outstanding performance for overall water splitting.