Photocatalytic Proton Reduction by a Computationally Identified, Molecular Hydrogen-Bonded Framework

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Aitchison, Catherine ORCID: 0000-0003-1437-8314, Kane, Christopher, McMahon, David P, Spackman, Peter, Wang, xiaoyan, Wilbraham, Liam, Pulido, Angeles, Chen, linjiang, Clowes, Rob, Little, Marc et al (show 4 more authors) , Zwijnenbur, Martijn A, Sprick, Reiner, Day, Graeme M and Cooper, Andrew ORCID: 0000-0003-0201-1021 (2020) Photocatalytic Proton Reduction by a Computationally Identified, Molecular Hydrogen-Bonded Framework. Journal of Materials Chemistry A, 2020 (15). pp. 7158-7170.

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Abstract

We show that a hydrogen-bonded framework, TBAP-α, with extended π-stacked pyrene columns has a sacrificial photocatalytic hydrogen production rate of up to 3108 µmol g-1 h-1. This is the highest activity reported for a molecular organic crystal. By comparison, a chemically-identical but amorphous sample of TBAP was 20–200 times less active, depending on the reaction conditions, showing unambiguously that crystal packing in molecular crystals can dictate photocatalytic activity. Crystal structure prediction (CSP) was used to predict the solid-state structure of TBAP and other functionalised, conformationally-flexible pyrene derivatives. Specifically, we show that energy-structure-function (ESF) maps can be used to identify molecules such as TBAP that are likely to form extended pi-stacked columns in the solid state. This opens up a methodology for the a priori computational design of molecular organic photocatalysts and other energy-relevant materials, such as organic electronics.

Item Type:	Article
Uncontrolled Keywords:	7 Affordable and Clean Energy
Depositing User:	Symplectic Admin
Date Deposited:	24 Jun 2020 10:57
Last Modified:	17 Mar 2024 07:42
DOI:	10.1039/d0ta00219d
Related URLs:	Author Publisher
URI:	https://livrepository.liverpool.ac.uk/id/eprint/3090695

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• Photocatalytic proton reduction by a computationally identified, molecular hydrogen-bonded framework. (deposited 19 Mar 2020 12:08)
  • Photocatalytic Proton Reduction by a Computationally Identified, Molecular Hydrogen-Bonded Framework. (deposited 24 Jun 2020 10:57) [Currently Displayed]