Pd@CuInPS Core-Shell Nanospheres with Exceptional Hydrogen Evolution Capability and Stability in Both Alkaline and Acidic Media under Large Current Density Exceeding 1000 mA cm.

By combining Pd with 2D layered crystal CuInPS (CIPS) via laser irradiation in liquids, low-loading Pd@CIPS core-shell nanospheres are fabricated as an efficient and robust electrocatalysts for HER in both alkaline and acidic media under large current density (⩾1000 mA cm). Pd@CIPS core-shell nanosphere has two structural features, i) the out-shell is the nanocomposite of PdH and PdInH, and ii) there is a kind of dendritic structure on the surface of nanospheres, while the dendritic structure porvides good gas desorption pathway and cause the Pd@CIPS system to maintain higher HER activity and stability than that of commercial Pt/C under large current densities. Pd@CIPS exhibits very low overpotentials of -218 and -313 mV for the large current density of 1000 mA cm, and has a small Tafel slope of 29 and 63 mV dec in 0.5 m HSO and 1 m KOH condition, respectively. Meanwhile, Pd@CIPS has an excellent stability under -10 and -500 mA cm current densities and 50 000 cycles cyclic voltammetry tests in 0.5 m HSO and 1 m KOH, respectively, which being much superior to that of commercial Pt/C. Density functional theory (DFT) reveals that engineering electronic structure of PdH and PdInH nanostructure can strongly weaken the Pd─H bonding.