| Summary: | Abstract Presented are the theoretical calculation and experimental studies of a Ti3C2Tx MXene‐based nanohybrid with simultaneous Nb doping and surface transition metal alloy modification. Guided by the density functional theory calculation, the Nb doping can move up the Fermi energy level to the conduction band, thus enhancing the electronic conductivity. Meanwhile, the surface modification by Ni/Co alloy can moderate the surface M–H affinity, which will further enhance the hydrogen evolution reaction (HER) activity. A series of Ni/Co alloy attached on Nb‐doped Ti3C2Tx MXene nanohybrids (denoted as NiCo@NTM) are successfully prepared. As expected, the Ni0.9Co0.1@ NTM nanohybrids present an extraordinary HER activity in alkaline solution, which only needs an overpotential (η) of 43.4 mV to reach the current density of 10 mA cm−2 in 1 m KOH solution and shows good stability. The performance of the Ni0.9Co0.1@ NTM nanohybrids is comparable to the commercial 10% Pt/C electrode (34.4 mV@10 mA cm−2) and is better than most state‐of‐the‐art Pt‐free HER catalysts. Inspired by the facile synthesis process and chemical versatility of both MXene and transition metal alloys, the nanohybrids reported here are promising non‐noble metal electrocatalysts for water–alkali electrolysis.
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