期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 11, 期 10, 页码 3941-3946出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c01196
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资金
- NSFC [21590811, 21777167, 21827809]
- National Key R&D Program of China [2018YFA0209302]
- Strategic Priority Research Program of Chinese Academy of Sciences [XDB36000000]
Despite the fact that proton-coupled electron transfer (PCET) has been hypothesized to play a pivotal role in the power conversion efficiency (PCE) of TiO2-based solar-energy applications, the specific relationship between the intrinsic nature of visible-light (Vis)-driven PCET reactions and limited PCE gains has not yet been well revealed. Here we studied the detailed kinetics of reactions between various alcohols and radicals ((Bu3ArO center dot)-Bu-t/TEMPO) on a TiO2 photocatalyst under dye-sensitization Vis irradiation versus direct ultraviolet (UV) irradiation. We found that the rates of Vis-driven reactions were much slower than those of UV-driven reactions under identical light intensity. A similar phenomenon was observed under the off-line dark-reaction conditions in which TiO2 was prereduced by alcohols. The rapid formation and difficult breakage of the stable Ti-H intermediate were proposed to account for the slowed-down PCET effect. This finding revealed an inherent bottleneck in Vis-driven energy conversion applications.
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