Oligoethylene glycol side chains increase charge generation in organic semiconductor nanoparticles for enhanced photocatalytic hydrogen evolution
File(s)
Accepted version
Author(s)
Type
Journal Article
Abstract
Organic semiconductor nanoparticles (NPs) composed of an electron donor/acceptor (D/A) semiconductor blend have recently emerged as an efficient class of hydrogen-evolution photocatalysts. It is demonstrated that using conjugated polymers functionalized with (oligo)ethylene glycol side chains in NP photocatalysts can greatly enhance their H2-evolution efficiency compared to their nonglycolated analogues. The strategy is broadly applicable to a range of structurally diverse conjugated polymers. Transient spectroscopic studies show that glycolation facilitates charge generation even in the absence of a D/A heterojunction, and further suppresses both geminate and nongeminate charge recombination in D/A NPs. This results in a high yield of photogenerated charges with lifetimes long enough to efficiently drive ascorbic acid oxidation, which is correlated with greatly enhanced H2-evolution rates in the glycolated NPs. Glycolation increases the relative permittivity of the semiconductors and facilitates water uptake. Together, these effects may increase the high-frequency relative permittivity inside the NPs sufficiently, to cause the observed suppression of exciton and charge recombination responsible for the high photocatalytic activities of the glycolated NPs.
Date Issued
2021-11-26
Date Acceptance
2021-10-01
Citation
Advanced Materials, 2021, 34 (22), pp.1-9
ISSN
0935-9648
Publisher
Wiley
Start Page
1
End Page
9
Journal / Book Title
Advanced Materials
Volume
34
Issue
22
Copyright Statement
© 2021 Wiley-VCH GmbH
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000722551100001&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Multidisciplinary
Chemistry, Physical
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Physics, Applied
Physics, Condensed Matter
Chemistry
Science & Technology - Other Topics
Materials Science
Physics
hydrogen
nanoparticles
organic semiconductors
photocatalysts
solar fuels
POLYMER PHOTOCATALYSTS
DIELECTRIC-CONSTANT
CONJUGATED POLYMERS
WATER
EFFICIENT
MOBILITY
ENERGY
TIO2
Publication Status
Published
Article Number
ARTN 2105007
Date Publish Online
2021-10-29