Excited-state and charge-carrier dynamics in binary conjugated polymer dots towards efficient photocatalytic hydrogen evolution

Aqueous dispersed conjugated polymer dots (Pdots) have shown promising application in photocatalytic hydrogen evolution. To efficiently extract photogenerated charges from type-II heterojunction Pdots for hydrogen evolution, the mechanistic study of photophysical processes is essential for Pdot opti...

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Published in:Physical chemistry chemical physics : PCCP 2023-01, Vol.25 (4), p.2935-2945
Main Authors: Liu, Aijie, Wang, Sicong, Song, Hongwei, Liu, Yawen, Gedda, Lars, Edwards, Katarina, Hammarström, Leif, Tian, Haining
Format: Article
Language:English
Subjects:
Absorption spectroscopy
Carrier recombination
Charge efficiency
Charge transfer
Current carriers
Energy transfer
Excitation
Heterojunctions
Hydrogen
Hydrogen evolution
Optimization
Photocatalysis
Photoluminescence
Polymers
Spectrum analysis
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Summary:Aqueous dispersed conjugated polymer dots (Pdots) have shown promising application in photocatalytic hydrogen evolution. To efficiently extract photogenerated charges from type-II heterojunction Pdots for hydrogen evolution, the mechanistic study of photophysical processes is essential for Pdot optimization. Within this work, we use a PFODTBT donor (D) polymer and an ITIC small molecule acceptor (A) as a donor/acceptor (D/A) model system to study their excited states and charge/energy transfer dynamics via steady-state and time-resolved photoluminescence spectroscopy, respectively. Charge-carrier generation and the recombination dynamics of binary Pdots with different D/A ratios were followed using femtosecond transient absorption spectroscopy. A significant spectral relaxation of photoluminescence was observed for individual D Pdots, implying an energetic disorder by nature. However, this was not seen for charge carriers in binary Pdots, probably due to the ultrafast charge generation process at an early time (
ISSN:1463-9076
1463-9084
1463-9084
DOI:10.1039/d2cp04204e