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. ORCID: https://orcid.org/0000-0002-1341-1541 and Tang, Junwang 2018. Bandgap engineering of organic semiconductors for highly efficient photocatalytic water splitting. Advanced Energy Materials 8 (24) , -. 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 Advanced Research Computing @ Cardiff (ARCCA) Cardiff Catalysis Institute (CCI)
Publisher:	Wiley
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:	05 May 2023 18:53
URI:	https://orca.cardiff.ac.uk/id/eprint/115400

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