Structurally Diverse Covalent Triazine-Based Framework Materials for Photocatalytic Hydrogen Evolution from Water

Christian B Meier; Rob Clowes; Enrico Berardo; Kim E Jelfs; Martijn A Zwijnenburg; Reiner Sebastian Sprick; Andrew I Cooper

doi:10.1021/acs.chemmater.9b02825

Structurally Diverse Covalent Triazine-Based Framework Materials for Photocatalytic Hydrogen Evolution from Water

Chem Mater. 2019 Nov 12;31(21):8830-8838. doi: 10.1021/acs.chemmater.9b02825. Epub 2019 Sep 27.

Authors

Christian B Meier¹, Rob Clowes¹, Enrico Berardo², Kim E Jelfs², Martijn A Zwijnenburg³, Reiner Sebastian Sprick¹, Andrew I Cooper¹

Affiliations

¹ Department of Chemistry and Materials Innovation Factory, University of Liverpool, 51 Oxford Street, Liverpool L7 3NY, U.K.
² Department of Chemistry, Molecular Sciences Research Hub, Imperial College London, White City Campus, Wood Lane, London W12 0BZ, U.K.
³ Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, U.K.

Abstract

A structurally diverse family of 39 covalent triazine-based framework materials (CTFs) are synthesized by Suzuki-Miyaura polycondensation and tested as hydrogen evolution photocatalysts using a high-throughput workflow. The two best-performing CTFs are based on benzonitrile and dibenzo[b,d]thiophene sulfone linkers, respectively, with catalytic activities that are among the highest for this material class. The activities of the different CTFs are rationalized in terms of four variables: the predicted electron affinity, the predicted ionization potential, the optical gap, and the dispersibility of the CTFs particles in solution, as measured by optical transmittance. The electron affinity and dispersibility in solution are found to be the best predictors of photocatalytic hydrogen evolution activity.