Tuning the Electronic Bandgap of Graphdiyne by H‐Substitution to Promote Interfacial Charge Carrier Separation for Enhanced Photocatalytic Hydrogen Production

• DOI: 10.1002/adfm.202100994
• Publication Date: 2021-03-30T07:50:00Z
• Authors: Jian Li; Amine Slassi; Xu Han; David Cornil; Minh‐Huong Ha‐Thi; Thomas Pino; Damien P. Debecker; Christophe Colbea...; Jordi Arbiol; Jérôme Cornil; Mohamed Nawfal Gh...
• Keywords: Charge carrier; Visible spectrum

Abstract Graphdiyne (GDY), which features a highly π‐conjugated structure, direct bandgap, and high charge carrier mobility, presents the major requirements for photocatalysis. Up to now, all photocatalytic studies are performed without paying too much attention on GDY bandgap (1.1 eV at G 0 W many‐body theory level). Such narrow is not suitable band alignment between other semiconductors, making it difficult achieve efficient photogenerated separation. Herein, first time, demonstrated that tuning electronic of via H‐substitution (H‐GDY) promotes interfacial separation improves H 2 evolution. The H‐GDY exhibits an increased energy ( ≈ 2.5 eV) exploitable conduction minimum valence maximum edges. As representative semiconductor, TiO hybridized with both fabricate heterojunction. Compared GDY/TiO , H‐GDY/TiO heterojunction leads remarkable enhancement generation by 1.35 times under UV–visible illumination (6200 µ mol h −1 g ) four visible light (670 ). attributed efficiently electron hole separation, as supported density functional calculations.