A dynamic surface reconstruction of oxide electrocatalysts in alkaline media is widely observed especially for layered double hydroxide (LDH), but little is known about how to promote the reconstruction toward desired surfaces for improved oxygen evolution reaction (OER). Here, surface reconstruction of NiFe LDH nanosheets is successfully induced to a higher degree via in situ sulfur doping than that by natural electrochemical activation. Theoretical calculations, operando Raman, and various ex situ characterizations reveal the S anion‐induced effect can lower the energy barrier and facilitate the phase transformation into highly active S‐doped oxyhydroxides. The generated S‐NixFeyOOH can optimize the intermediate adsorption and facilitate the OER kinetics. The reconstructed S‐oxyhydroxides catalyst presents superior OER activity and long‐term durability compared to undoped ones. This work provides a structure–composition–activity relationship during the in situ surface restructuring of NiFe LDH pre‐catalysts.
Suitable electrocatalysts for industrial water splitting can veritably promote practical hydrogen applications. Rational surface design is exceptionally significant for electrocatalysts to bridge the gap between fundamental science and industrial expectation in water splitting. Here, Pt‐quantum‐dot‐modified sulfur‐doped NiFe layered double hydroxides (Pt@S–NiFe LDHs) are designed with eximious catalytic activity toward hydrogen evolution reaction (HER) under industrial condition. Benefiting from enhanced binding energy, mass transfer, and hydrogen release, Pt@S–NiFe LDHs exhibit outstanding activity in HER at high current densities. Notably, it obtains an impressively low overpotential of 71 mV and long‐term stability of 200 h at 100 mA cm−2, exceeding commercial 40% Pt/C and most reported Pt‐based electrocatalysts. Its mass activity is 2.7 times higher than that of 40% Pt/C with an overpotential of 100 mV. Furthermore, at industrial temperature (65 °C), the electrolyzer based on Pt@S–NiFe LDH needs just 1.62 V to reach the current density of 100 mA cm−2, superior to that of the commercial one of 40% Pt/C//IrO2. This work provides rational ideas to develop electrocatalysts with exceptional performance for industrial high‐temperature water splitting at high current densities.
Insufficient catalytic activity and self-restacking of 2D MXenes during catalytic processes would lead to limited number of active sites, sluggish ionic kinetics and poor durability, extremely restricting its application in...
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