Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 114, Issue 9, Pages 4208-4214Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp909993w
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Funding
- EPSRC
- Engineering and Physical Sciences Research Council [EP/F00270X/1] Funding Source: researchfish
- EPSRC [EP/F00270X/1] Funding Source: UKRI
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We report on the mechanism of water splitting by TiO2 in the absence of chemical scavengers in a fully functional photoelectrochemical (PEC) cell. The application of a positive potential to a nanocrystalline-TiO2 film is shown to lead to the formation of long-lived holes which oxidize water on the milliseconds time scale. These first time-resolved Studies of a nanocrystalline-TiO2 (nc-TiO2) film in a complete PEC cell also showed that all of the long-lived photoholes go on to generate O-2, and that there are no major branching inefficiencies in the catalysis itself, which appears to be operating at efficiencies close to 100%. The overall quantum yield of oxygen production under pulsed illumination (355 nm) was found to be similar to 8% at excitation densities of 4.4 photons per particle. Under all conditions examined, electron-hole recombination was found to be the dominant loss pathway.
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