Tunable organic photocatalysts for visible-light-driven hydrogen evolution

Sprick, R. S., Jiang, J.-X., Bonillo, B., Ren, S., Ratvijitvech, T., Guiglion, P., Zwijnenburg, M. A., Adams, D. J. and Cooper, A. I. (2015) Tunable organic photocatalysts for visible-light-driven hydrogen evolution. Journal of the American Chemical Society, 137(9), pp. 3265-3270. (doi: 10.1021/ja511552k) (PMID:25643993)

Abstract

Photocatalytic hydrogen production from water offers an abundant, clean fuel source, but it is challenging to produce photocatalysts that use the solar spectrum effectively. Many hydrogen-evolving photocatalysts are active in the ultraviolet range, but ultraviolet light accounts for only 3% of the energy available in the solar spectrum at ground level. Solid-state crystalline photocatalysts have light absorption profiles that are a discrete function of their crystalline phase and that are not always tunable. Here, we prepare a series of amorphous, microporous organic polymers with exquisite synthetic control over the optical gap in the range 1.94–2.95 eV. Specific monomer compositions give polymers that are robust and effective photocatalysts for the evolution of hydrogen from water in the presence of a sacrificial electron donor, without the apparent need for an added metal cocatalyst. Remarkably, unlike other organic systems, the best performing polymer is only photoactive under visible rather than ultraviolet irradiation.

• Item Type: Articles
• Additional Information: We thank EPSRC (EP/C511794/1) for funding. M.A.Z. acknowledges EPSRC for a fellowship (EP/I004424/1). We thank F. Armstrong, M. Bojdys, C. Butchosa, A. Cowan, J. Walsh, G. Cheng, and B. Kiss for helpful discussions. T. Hasell is acknowledged for help with TGA measurements and with SEM. We acknowledge computational time on HECToR/ARCHER, the United Kingdom’s national high-performance computing (HPC) service, via our membership of the United Kingdom’s HPC Materials Chemistry Consortium, which is funded by EPSRC grants EP/F067496/1 and EP/L000202/1, and also the EPSRC United Kingdom National Service for Computational Chemistry Software (NSCCS) at Imperial College London.
• Status: Published
• Refereed: Yes
• Glasgow Author(s) Enlighten ID: Adams, Dave
• Authors: Sprick, R. S., Jiang, J.-X., Bonillo, B., Ren, S., Ratvijitvech, T., Guiglion, P., Zwijnenburg, M. A., Adams, D. J., and Cooper, A. I.
• College/School: College of Science and Engineering > School of Chemistry
• Journal Name: Journal of the American Chemical Society
• Publisher: American Chemical Society
• ISSN: 0002-7863
• ISSN (Online): 1520-5126
• Published Online: 03 February 2015
• Copyright Holders: Copyright © 2015 American Chemical Society
• First Published: First published in Journal of the American Chemical Society 137(9): 3265-3270
• Publisher Policy: Reproduced under a creative Commons license