Abstract
By combining Pd with 2D layered crystal CuInP2S6 (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 (⩾1000mAcm-2). Pd@CIPS core-shell nanosphere has two structural features, i) the out-shell is the nanocomposite of PdHx and PdInHx, 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 -313mV for the large current density of 1000mAcm-2, and has a small Tafel slope of 29 and 63mVdec-1 in 0.5mH2SO4 and 1mKOH condition, respectively. Meanwhile, Pd@CIPS has an excellent stability under -10 and -500mAcm-2 current densities and 50000 cycles cyclic voltammetry tests in 0.5mH2SO4 and 1mKOH, respectively, which being much superior to that of commercial Pt/C. Density functional theory (DFT) reveals that engineering electronic structure of PdHx and PdInHx nanostructure can strongly weaken the Pd─H bonding.
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