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Title: Ultrathin‐Film Titania Photocatalyst on Nanocavity for CO 2 Reduction with Boosted Catalytic Efficiencies

Photocatalytic CO2reduction with water to hydrocarbons represents a viable and sustainable process toward greenhouse gas reduction and fuel/chemical production. Development of more efficient catalysts is the key to mitigate the limits in photocatalytic processes. Here, a novel ultrathin‐film photocatalytic light absorber (UFPLA) with TiO2films to design efficient photocatalytic CO2conversion processes is created. The UFPLA structure conquers the intrinsic trade‐off between optical absorption and charge carrier extraction efficiency, that is, a solar absorber should be thick enough to absorb majority of the light allowable by its bandgap but thin enough to allow charge carrier extraction for reactions. The as‐obtained structures significantly improve TiO2photocatalytic activity and selectivity to oxygenated hydrocarbons than the benchmark photocatalyst (Aeroxide P25). Remarkably, UFPLAs with 2‐nm‐thick TiO2films result in hydrocarbon formation rates of 0.967 mmol g−1h−1, corresponding to 1145 times higher activity than Aeroxide P25. This observation is confirmed by femtosecond transient absorption spectroscopic experiments where longer charge carrier lifetimes are recorded for the thinner films. The current work demonstrates a powerful strategy to control light absorption and catalysis in CO2conversion and, therefore, creates new and transformative ways of converting solar energy and greenhouse gas to alcohol fuels/chemicals.

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Author(s) / Creator(s):
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Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Global Challenges
Medium: X
Sponsoring Org:
National Science Foundation
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