Highly Efficient and Stable Iridium Oxygen Evolution Reaction Electrocatalysts Based on Porous Nickel Nanotube Template Enabling Tandem Devices with Solar‐to‐Hydrogen Conversion Efficiency Exceeding 10%

Abstract Ir is one of the most efficient oxygen evolution reaction (OER) catalysts; however, it is also one of the rarest and most expensive elements. Therefore, it is highly desirable to develop Ir catalysts with nanostructures that reduce Ir consumption by maximizing the surface‐to‐volume ratio without limiting the mass transport of reactants and products of reactions. Ir OER catalysts on a template that consisted of porous nanotubes (PNTs) based on Ni are fabricated. The Ir/Ni PNTs offer multiple benefits, including high catalytic performance (potential of 1.500 V vs. reversible hydrogen electrode (RHE) at an operating current density of 10 mA cm⁻² and Tafel slope of 44.34 mV decade⁻¹), minimal use of Ir (mass activity of 3273 A g⁻¹ at 1.53 V vs RHE), and facile mass transport through the NT‐sidewall pores (stable operation for more than 10 h). The Ir/Ni PNTs are also applied to a tandem device, consisting of a Cu(In,Ga)Se₂‐based photocathode and halide perovskite photovoltaic cell, for unassisted water splitting. A solar‐to‐hydrogen conversion efficiency that exceeded 10% is also demonstrated, which is nearly 1% point greater than when a planar Ir film is used as the anode instead of Ir/Ni PNTs.