Interface Engineering of a CoOx/Ta₃N₅ Photocatalyst for Unprecedented Water Oxidation Performance under Visible‐Light‐Irradiation

Cocatalysts have been extensively used to promote water oxidation efficiency in solar-to-chemical energy conversion, but the influence of interface compatibility between semiconductor and cocatalyst has been rarely addressed. Here we demonstrate a feasible strategy of interface wettability modification to enhance water oxidation efficiency of the state-of-the-art CoO(x)/Ta3N5 system. When the hydrophobic feature of a Ta3N5 semiconductor was modulated to a hydrophilic one by in situ or ex situ surface coating with a magnesia nanolayer (2-5 nm), the interfacial contact between the hydrophilic CoO(x) cocatalyst and the modified hydrophilic Ta3N5 semiconductor was greatly improved. Consequently, the visible-light-driven photocatalytic oxygen evolution rate of the resulting CoO(x)/MgO(in)-Ta3N5 photocatalyst is ca. 23 times that of the pristine Ta3N5 sample, with a new record (11.3%) of apparent quantum efficiency (AQE) under 500-600 nm illumination.