Coupling Red‐to‐blue Upconversion Organic Microcrystals with Cd0.5Zn0.5S for Efficient and Durable Photocatalytic Hydrogen Production

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For semiconductor photocatalysts with excellent performance in solar H 2 production, broadening the utilization of solar irradiation is highly necessary to further improve the solar conversion efficiency. Herein, we combined a Cd 0.5 Zn 0.5 S photocatalyst with DPA/PdTPTBP microcrystals capable of red‐to‐blue photon upconversion, realizing substantial performance enhancement and an apparent quantum yield of 0.16% for H 2 production driven by sub‐bandgap photons (600∼650 nm). Meanwhile, this system could smoothly work with H 2 production rate of 1.40 mmol g −1 h −1 for as long as 40 hours under 200 mW/cm 2 irradiation with only 3% attenuation of photocatalytic activity. Moreover, the O 2 ‐barrier property of DPA/PdTPTBP microcrystals assures that photocatalytic H 2 production remains effective in the presence of 10% O 2 by volume, which offers an opportunity for the photocatalytic application in O 2 ‐enriched environments. The combination of O 2 ‐resistant upconversion microcrystals and semiconductor catalysts is the most successful solution for the construction of TTA‐UC‐based photocatalytic H 2 production system so far. The present study provides a clear guideline for designing new TTA‐UC‐based photocatalytic systems.