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Bandgap engineering of organic semiconductors for highly efficient photocatalytic water splitting

Wang, Yiou, Silveri, Fabrizio, Bayazit, Mustafa K., Ruan, Qiushi, Li, Yaomin, Xie, Jijia, Catlow, C. Richard A. and Tang, Junwang 2018. Bandgap engineering of organic semiconductors for highly efficient photocatalytic water splitting. Advanced Energy Materials 8 (24) , 1801084. 10.1002/aenm.201801084

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Abstract

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 H2 and O2 evolution at ambient conditions (420 nm < λ < 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.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: Wiley-VCH Verlag
ISSN: 1614-6832
Funders: Leverhulme Trust, EPSRC, Royal Society
Date of First Compliant Deposit: 1 October 2018
Date of Acceptance: 28 June 2018
Last Modified: 29 Jun 2019 21:45
URI: http://orca-mwe.cf.ac.uk/id/eprint/115400

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