Efficient separation of photogenerated electrons and holes, and associated surface reactions, is a crucial aspect of efficient semiconductor photocatalytic systems employed for photocatalytic hydrogen production. A new CoO x /TiO 2 /Pt photocatalyst produced by template‐assisted atomic layer deposition is reported for photocatalytic hydrogen production on Pt and CoO x dual cocatalysts. Pt nanoclusters acting as electron collectors and active sites for the reduction reaction are deposited on the inner surface of porous TiO 2 nanotubes, while CoO x nanoclusters acting as hole collectors and active sites for oxidation reaction are deposited on the outer surface of porous TiO 2 nanotubes. A CoO x /TiO 2 /Pt photocatalyst, comprising ultra‐low concentrations of noble Pt (0.046 wt %) and CoO x (0.019 wt %) deposited simultaneously with one atomic layer deposition cycle, achieves remarkably high photocatalytic efficiency (275.9 μmol h −1 ), which is nearly five times as high as that of pristine TiO 2 nanotubes (56.5 μmol h −1 ). The highly dispersed Pt and CoO x nanoclusters, porous structure of TiO 2 nanotubes with large specific surface area, and the synergetic effect of the spatially separated Pt and CoO x dual cocatalysts contribute to the excellent photocatalytic activity.
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