Realizing high-efficiency carrier separation in 3D hierarchical carbon nitride nanosheets via intramolecular donor-acceptor motifs strategy. (September 2022)

• Record Type: Journal Article
• Authors: Xing, W.; Shao, W.; Tian, L.; Zhang, Y.; Yang, J.; Zhou, H.; Han, J.; Wu, G.; Chen, G.
• Is Part Of: Materials today chemistry. Volume 25(2022)
• Publication Date: 2022-09
• Subjects: g-C3N4 -- Donor-acceptor -- Photocatalytic -- Hydrogen evolution; Chemistry -- Periodicals; Materials -- Research -- Periodicals; Materials science -- Periodicals; Chemistry; Materials -- Research; Electronic journals; Periodicals; 660.282
• DOI: 10.1016/j.mtchem.2022.100977
• Languages: English
• ISSNs: 2468-5194

Abstract

Abstract: The insufficient visible light responsive region and fast charge recombination probability are still the key obstacles for designing high-performance photocatalytic system. Herein, a "One Stone, Two Birds" strategy was reported in three-dimensional (3D) hierarchical graphitic carbon nitride (g-C3 N4 ) nanosheet with intramolecular donor-acceptor (D-A) motifs (3D CN) photocatalyst, which solved two urgent problems simultaneously. The 3D hierarchical nanosheets structure endowed 3D CN with abundantly exposed reaction active sites and cross-plane diffusion channels. The formation of internal D-A system facilitated the light absorption and accelerated the transfer and separation of charge carriers. Furthermore, the introducing of D-A motifs optimized the bandgap of g-C3 N4 and negative-shifted conduction band position. The as-prepared 3D CN showed excellent visible-light photocatalytic H2 performance, with H2 evolution rate of 2521.2 μmol h −1 /g, which was six times higher than the pristine CN. This outstanding performance was ascribed to the synergistic effect of 3D hierarchical nanosheets structure and intramolecular D-A motifs. This current work provides a novel insight to design and construct of 3D hierarchical CN nanostructures with D-A motifs simultaneously, which can be further promising applications for clean and sustainable energy conversion. Graphical abstract: Image 1 Highlights: 3D hierarchical g-C3 N4 nanosheet with intramolecular donor-acceptor (D-A) motifs is fabricated. The photocatalytic H2 evolution rate over 3D CN has a 6-fold increase over primal CN. The D-A motifs optimize bandgap structures and enhance the charge separation efficiency. The synergistic effect of 3D hierarchical nanosheets and D-A motifs contributes to the high H2 activity.