Realizing the Tailored Catalytic Performances on Atomic Pt-Promoted Transition Metal Moieties Implanted Layered Double Hydroxides for Water Electrolysis.

High-performance production of green hydrogen gas is necessary to develop renewable energy generation technology and to safeguard the living environment. This study reports a controllable engineering approach to tailor the structure of nickel-layered double hydroxides via doped and absorbed platinum single atoms (Pt SA ) promoted by low electronegative transition metal (Mn, Fe) moieties (Pt SA -Mn,Fe-Ni LDHs). We explore that the electron donation from neighboring transition metal moieties results in the well-adjusted d -band center with the low valence states of Pt SA(doped) and Pt SA(ads.) , thus optimizing adsorption energy to effectively accelerate the H 2 release. Meanwhile, a tailored local chemical environment on transition metal centers with unique charge redistribution and high valence states functions as the main center for H 2 O catalytic dissociation into oxygen. Therefore, the Pt SA -Mn,Fe-Ni LDH material possesses a small overpotential of 42 and 288 mV to reach 10 mA·cm -2 for hydrogen and oxygen evolution, respectively, superior to most reported LDH-based catalysts. Additionally, the mass activity of Pt SA -Mn,Fe-Ni LDHs proves to be 15.45 times higher than that of commercial Pt-C. The anion exchange membrane electrolyzer stack of Pt SA -Mn,Fe-Ni LDHs (+,-) delivers a cell voltage of 1.79 V at 0.5 A·cm -2 and excellent durability over 600 h. This study presents a promising electrocatalyst for a practical water splitting process.