Synthesis of P‐(NiCo)CO3/TiO2/Ti Self‐Supported Electrode with High Catalytic Activity and Stability for Hydrogen Evolution

Abstract Hydrogen is considered an ideal clean energy due to its high mass‐energy density, and only water is generated after combustion. Water electrolysis is a sustainable method of obtaining a usable amount of pure hydrogen among the various hydrogen production methods. However, its development is still limited by applying expensive noble metal catalysts. Here, the dissolution‐recrystallization process of TiO 2 nanotube arrays in water with the hydrothermal reaction of a typical nickel‐cobalt hydroxide synthesis process followed by phosphating to prepare a self‐supported electrode with (NiCo)CO 3 /TiO 2 heterostructure named P‐(NiCo)CO 3 /TiO 2 /Ti electrode is combined. The electrode exhibits an ultra‐low overpotential of 31 mV at 10 mA cm −2 with a Tafel slope of 46.2 mV dec −1 in 1 m KOH and maintained its stability after running for 500 h in 1 m KOH. The excellent catalytic activity can be attributed to the structure of nanotube arrays with high specific surface area, superhydrophilicity, and super aerophobicity on the electrode surface. In addition, the uniform (NiCo)CO 3 /TiO 2 heterostructure also accelerates the electron transfer on the electrode surface. Finally, DFT calculations demonstrate that phosphating also improves the ΔG H* and ΔG H2O of the electrode. The synthesis strategy also promotes the exploration of catalysts for other necessary electrocatalytic fields.