Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 19, Pages 5320-5324Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201713102
Keywords
hole scavenging; methanol; photocatalysis; photoexcited hole dynamics; ultrafast transient absorption spectroscopy
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Funding
- MOST [2016YFA0200602, 2017YFA0303500]
- NSFC [21573211, 21633007, 21421063, 21790350]
- Fundamental Research Funds for the Central Universities of China [WK2340000063]
- CAS [2016HSC-IU003]
- Anhui Initiative in Quantum Information Technologies [AHY090000]
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An experimental scrutiny of the photoexcited hole dynamics in a prototypical system is presented in which hole-scavenging methanol molecules are chemisorbed on a graphitic carbon nitride (g-C3N4) substrate. A set of comparison and control experiments by means of femtosecond time-resolved transient absorption (fs-TA) spectroscopy were conducted. The elusive reverse hole transfer (RHT) process was identified, which occurs on a timescale of a few hundred picoseconds. The critical role of interfacially chemisorbed methoxy (instead of methanol) as the dominant species responsible for hole scavenging was confirmed by a control experiment using protonated g-C3N4 as the substrate. A hot-hole transfer effect was revealed by implementing different interband photoexcitation scenarios. The RHT rate is the key factor governing the hole-scavenging ability of different hole scavengers.
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