Journal
ADVANCED ENERGY MATERIALS
Volume 8, Issue 24, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201801084
Keywords
bandgap; organic semiconductors; photocatalytic; polymers; water splitting
Categories
Funding
- CSC
- Leverhulme Trust [RPG-2012-582, RPG-2017-122]
- EPSRC [EP/N009533/1, EP/F067496]
- Royal Society-Newton Advanced Fellowship grants [NA170422]
- Cardiff University School of Chemistry
- EPSRC [EP/N009533/1] Funding Source: UKRI
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The bandgap engineering of semiconductors, in particular low-cost organic/polymeric photocatalysts could directly influence their behavior in visible photon harvesting. However, an effective and rational pathway to stepwise change of the bandgap of an organic/polymeric photocatalyst is still very challenging. An efficient strategy is demonstrated to tailor the bandgap from 2.7 eV to 1.9 eV of organic photocatalysts by carefully manipulating the linker/terminal atoms in the chains via innovatively designed polymerization. These polymers work in a stable and efficient manner for both H-2 and O-2 evolution at ambient conditions (420 nm < lambda < 710 nm), exhibiting up to 18 times higher hydrogen evolution rate (HER) than a reference photocatalyst g-C3N4 and leading to high apparent quantum yields (AQYs) of 8.6%/2.5% at 420/500 nm, respectively. For the oxygen evolution rate (OER), the optimal polymer shows 19 times higher activity compared to g-C3N4 with excellent AQYs of 4.3%/1.0% at 420/500 nm. Both theoretical modeling and spectroscopic results indicate that such remarkable enhancement is due to the increased light harvesting and improved charge separation. This strategy thus paves a novel avenue to fabricate highly efficient organic/polymeric photocatalysts with precisely tunable operation windows and enhanced charge separation.
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