A computational survey of metal-free polyimide-based photocatalysts within the single-stranded polymer model

Jong Hun Park, Aloysius Soon, Ji Hwan Lee

Research output: Contribution to journalArticlepeer-review

4 Citations (Scopus)

Abstract

Eco-friendly production of hydrogen using the solar water-splitting reaction is one of the key technologies for clean energy generation. In this work, using hybrid density-functional theory calculations, we survey a number of isolated polyimide chains for prospective candidates as metal-free organic photocatalysts, given their known excellent thermal stability and chemical resistance. We evaluate their capability to split water following the three key requirements for a good photocatalyst: (1) proper HOMO/LUMO energy levels with respect to the water redox potential, (2) appropriate energy gap sizes for the maximum usability of visible light, and (3) the ability to separate the charge carriers (electron and hole) optimally. Using the well-reported graphitic carbon nitride (g-C3N4) as benchmark, we find that both PMDA-ODA and BTDA-ODA polyimides are most promising, with a favourable HOMO–LUMO energy gap and well-separated electron and hole localized on each monomer fragment of the polyimide strand. From our optical response calculations, these PMDA-ODA and BTDA-ODA polyimides are also found to be better absorbers of visible light than e.g. g-C3N4. This study will provide a good theoretical platform for optimizing the next-generation metal-free polymeric photocatalysts for hydrogen production from water under visible light.

Original languageEnglish
Article number111184
JournalMolecular Catalysis
Volume497
DOIs
Publication statusPublished - 2020 Dec

Bibliographical note

Publisher Copyright:
© 2020 Elsevier B.V.

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Process Chemistry and Technology
  • Physical and Theoretical Chemistry

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