Issue 1, 2022

Intramolecular π-conjugated channel expansion achieved by doping cross-linked dopants into carbon nitride frameworks for propelling photocatalytic hydrogen evolution and mechanism insight

Abstract

Developing modified carbon nitride (CN) with a multi-bonding mode remains a pivotal challenge for high-efficiency photocatalytic hydrogen evolution (PHE). Here, we fabricate a PYM-CN photocatalyst by doping pyrimethamine (PYM) in CN by a facile one-step polymerization method, which shows remarkably enhanced PHE performance in contrast with pure CN, because PYM as a cross-linked bridge in CN frameworks via a multi-bonding mode broadens the visible-light absorption range and expedites the transfer and separation of intramolecular photoproduced electron–hole pairs by π-conjugated channel expansion. Density functional theory (DFT) calculations reveal that this significant improvement is attributed to the orbital hybridization and delocalization effects resulting from the unique intramolecular cross-linked structure in PYM-CN. As expected, the PHE rate over the optimal PYM100-CN sample is about 11.6 times that of pure CN and the AQE value reaches up to 17.7% at 420 nm. Hence, this work provides a representative paradigm to exploit intramolecular cross-linked polymer photocatalysts with a multi-bonding mode for the high-efficiency PHE reaction or other photocatalytic application fields.

Graphical abstract: Intramolecular π-conjugated channel expansion achieved by doping cross-linked dopants into carbon nitride frameworks for propelling photocatalytic hydrogen evolution and mechanism insight

Supplementary files

Article information

Article type
Research Article
Submitted
05 Sep 2021
Accepted
21 Okt 2021
First published
22 Okt 2021

Inorg. Chem. Front., 2022,9, 60-69

Intramolecular π-conjugated channel expansion achieved by doping cross-linked dopants into carbon nitride frameworks for propelling photocatalytic hydrogen evolution and mechanism insight

C. Li, T. Zhou, M. Yan, S. Cheng, Y. Wang, J. Sun, G. Chen and H. Dong, Inorg. Chem. Front., 2022, 9, 60 DOI: 10.1039/D1QI01122G

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