共 30 条
Dynamics of Electron Transfers in Photosensitization Reactions of Zinc Porphyrin Derivatives
被引:0
作者:
Kim, Soohwan
[1
]
Kim, Taesoo
[1
]
Choi, Sunghan
[1
]
Son, Ho-Jin
[1
]
Kang, Sang Ook
[1
]
Shin, Jae Yoon
[1
]
机构:
[1] Korea Univ, Dept Adv Mat Chem, Sejong 30019, South Korea
来源:
MOLECULES
|
2023年
/
28卷
/
01期
基金:
新加坡国家研究基金会;
关键词:
Zn porphyrin;
TiO2;
electron transfer;
photosensitizer;
time-resolved spectroscopy;
CHARGE-TRANSFER;
DYE;
FLUORESCENCE;
REDUCTION;
STATE;
TIO2;
PHTHALOCYANINE;
PHOTOCATALYST;
PERFORMANCE;
SELECTIVITY;
D O I:
10.3390/molecules28010327
中图分类号:
Q5 [生物化学];
Q7 [分子生物学];
学科分类号:
071010 ;
081704 ;
摘要:
Photocatalytic systems for CO2 reduction operate via complicated multi-electron transfer (ET) processes. A complete understanding of these ET dynamics can be challenging but is key to improving the efficiency of CO2 conversion. Here, we report the ET dynamics of a series of zinc porphyrin derivatives (ZnPs) in the photosensitization reactions where sequential ET reactions of ZnPs occur with a sacrificial electron donor (SED) and then with TiO2. We employed picosecond time-resolved fluorescence spectroscopy and femtosecond transient absorption (TA) measurement to investigate the fast ET dynamics concealed in the steady-state or slow time-resolved measurements. As a result, Stern-Volmer analysis of fluorescence lifetimes evidenced that the reaction of photoexcited ZnPs with SED involves static and dynamic quenching. The global fits to the TA spectra identified much faster ET dynamics on a few nanosecond-time scales in the reactions of one-electron reduced species (ZnPs(center dot-)) with TiO2 compared to previously measured minute-scale quenching dynamics and even diffusion rates. We propose that these dynamics report the ET dynamics of ZnPs(center dot-) formed at adjacent TiO2 without involving diffusion. This study highlights the importance of ultrafast time-resolved spectroscopy for elucidating the detailed ET dynamics in photosensitization reactions.
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页数:10
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