Journal
ADVANCED MATERIALS
Volume 34, Issue 22, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202105007
Keywords
hydrogen; nanoparticles; organic semiconductors; photocatalysts; solar fuels
Categories
Funding
- Office of Sponsored Research (OSR) [OSR-2018-CRG/CCF-3079, OSR-2019-CRG8-4086 IED-OSR-2019-4454, OSR-2018-CRG7-3749]
- ERC Synergy Grant SC2 [610115]
- EUHorizon 2020 research and innovation program [952911]
- project BOOSTER, Horizon 2020 research and innovation program [862474]
- project RoLAFLEX
- EPSRC [EP/T026219/1]
- European Union [886664]
- KAUST
- EPSRC [EP/T026219/1] Funding Source: UKRI
- Marie Curie Actions (MSCA) [886664] Funding Source: Marie Curie Actions (MSCA)
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It has been found that incorporating conjugated polymers with ethylene glycol side chains into organic semiconductor nanoparticles can significantly enhance hydrogen-evolution efficiency. Glycolation promotes charge generation, reduces charge recombination, and ultimately boosts hydrogen-evolution rates in the nanoparticles.
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 H-2-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 H-2-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.
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