S-doped C3N5 derived from thiadiazole for efficient photocatalytic hydrogen evolution

Xinwei Guan, Mohammed Fawaz, Ranjini Sarkar, Chun Ho Lin, Zhixuan Li, Zhihao Lei, Panangattu Dharmarajan Nithinraj, Prashant Kumar, Xiangwei Zhang, Jae Hun Yang, Long Hu, Tom Wu, Sudip Chakraborty, Jiabao Yi, Ajayan Vinu

Research output: Journal article publicationJournal articleAcademic researchpeer-review

27 Citations (Scopus)

Abstract

Graphitic carbon nitrides (g-C3N4) with unique physicochemical properties are promising candidates for photocatalysis applications. However, pristine g-C3N4 often suffers from narrow absorption ranges and high carrier recombination rates, which result in mediocre catalytic performance. In this work, we prepare novel sulfur-doped high nitrogen containing carbon nitrides, C3N5 (SCNs), with a combined thiadiazole, triazole, and triazine framework by facile self-assembly of 5-amino-1,3,4-thiadiazole-2-thiol (5-ATDT). Their structural, morphological, and optical properties, and photocatalytic activities are investigated in detail. From density functional theory calculations and spectroscopic characterization studies, we construct thermodynamically stable molecular structures of SCNs composed of one triazole and two triazine moieties with small ratios of thiadiazole on the edge, in which the sulfur atoms are ionically connected with carbon/nitrogen atoms and gradually detached on increasing the calcination temperatures. Remarkably, the resultant SCNs exhibit a significantly enhanced H2-generation rate of 486 μmol g−1 h−1, about 60% higher than the average value derived from typical g-C3N4 synthesised by conventional precursors thanks to the enlarged light absorption range and enhanced charge carrier transfer rate. Our work provides a unique approach for designing novel sulfur-doped carbon nitrides with unprecedented functionalities.

Original languageEnglish
Pages (from-to)12837-12845
Number of pages9
JournalJournal of Materials Chemistry A
Volume11
Issue number24
DOIs
Publication statusPublished - 7 Feb 2023

ASJC Scopus subject areas

  • General Chemistry
  • Renewable Energy, Sustainability and the Environment
  • General Materials Science

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