TY - JOUR
T1 - S-doped C3N5 derived from thiadiazole for efficient photocatalytic hydrogen evolution
AU - Guan, Xinwei
AU - Fawaz, Mohammed
AU - Sarkar, Ranjini
AU - Lin, Chun Ho
AU - Li, Zhixuan
AU - Lei, Zhihao
AU - Nithinraj, Panangattu Dharmarajan
AU - Kumar, Prashant
AU - Zhang, Xiangwei
AU - Yang, Jae Hun
AU - Hu, Long
AU - Wu, Tom
AU - Chakraborty, Sudip
AU - Yi, Jiabao
AU - Vinu, Ajayan
N1 - Funding Information:
X. Guan and M. Fawaz contributed equally to this work. The authors would like to acknowledge Siddulu Naidu Talapaneni for helping with the SCN reaction path construction. R. S. and S. C would like to acknowledge the Center of Excellence in Materials and Manufacturing for Futuristic Mobility, IIT Madras for financial support and HRI Allahabad, and DST-SERB Funding (SRG/2020/001707) for the infrastructure. A. V. would like to acknowledge the Australian Research Council (ARC) for the Future Fellowship award (FT100100970) and a start-up grant from the University of Newcastle. J. Y. acknowledges the ARC grant support (DP220103045, LP210100436 and LP200201079).
Publisher Copyright:
© 2023 The Royal Society of Chemistry.
PY - 2023/2/7
Y1 - 2023/2/7
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85149695091&partnerID=8YFLogxK
U2 - 10.1039/d3ta00318c
DO - 10.1039/d3ta00318c
M3 - Journal article
AN - SCOPUS:85149695091
SN - 2050-7488
VL - 11
SP - 12837
EP - 12845
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
IS - 24
ER -