Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 116, Issue 21, Pages 10232-10237Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1901631116
Keywords
photocatalyst; defect engineering; metal-oxide interface; solar hydrogen production; oxygen vacancy
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Funding
- National Natural Science Foundation of China [U1305242, 21173044, 21373048, 21373050]
- Welch Foundation [F-1861]
- Sloan Research Foundation
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Close proximity between different catalytic sites is crucial for accelerating or even enabling many important catalytic reactions. Photooxidation and photoreduction in photocatalysis are generally separated from each other, which arises from the hole-electron separation on photocatalyst surface. Here, we show with widely studied photocatalyst Pt/TiO2 as a model, that concentrating abundant oxygen vacancies only at the metal-oxide interface can locate hole-driven oxidation sites in proximity to electron-driven reduction sites for triggering unusual reactions. Solar hydrogen production from aqueous-phase alcohols, whose hydrogen yield per photon is theoretically limited below 0.5 through conventional reactions, achieves an ultrahigh hydrogen yield per photon of 1.28 through the unusual reactions. We demonstrated that such defect engineering enables hole-driven CO oxidation at the Pt-TiO2 interface to occur, which opens up room-temperature alcohol decomposition on Pt nanoparticles to H-2 and adsorbed CO, accompanying with electron-driven proton reduction on Pt to H-2.
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