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The design of photocatalysts plays a central role in determining the photocatalytic H 2 yield. Here, we used a design strategy that is different from conventional methods to prepare our photocatalytic systems. Large porous carbon aerogels (CA) with rich surface areas were used to receive photogenerated electrons. TiO 2 quantum dots were used as photocatalysts and anchored on large porous CAs to form CA@TiO 2 systems. The H 2 yield of the optimized CA@TiO 2 composite is ∼2.1 mmol/g, ∼11 times higher than that of pure TiO 2 quantum dots. High-resolution X-ray photoelectron spectroscopy and high-angle annular dark-field scanning transmission electron microscopy demonstrate that the photogenerated electrons can be easily transferred from TiO 2 quantum dots to porous CAs. Thus, efficient charge separation can be realized for the succeeding highly efficient H 2 evolution. Our results here provide a different way from conventional methods to design photocatalytic systems with high H 2 yield.

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