Aromatic Ring-Coordinated g-C3N4 Nanotubes for Enhanced Photocatalytic H2 Evolution

Chongze Cai; Huaiyu Lu; Cheng Cheng; Wengao Zeng; Xiangjiu Guan; Liuhao Mao; Li Tian; Jinwen Shi; Liejin Guo

doi:10.1007/s12209-025-00454-0

Transactions of Tianjin University ›› 2025, Vol. 31 ›› Issue (6) :555 -566. DOI: 10.1007/s12209-025-00454-0

Research Article

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Aromatic Ring-Coordinated g-C₃N₄ Nanotubes for Enhanced Photocatalytic H₂ Evolution

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¹International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University, 710049, Xi’an, China

^a ccheng-xjtu@xjtu.edu.cn

^b xj-guan@mail.xjtu.edu.cn

^c jinwen_shi@mail.xjtu.edu.cn

Chongze Cai

Chongze Cai is currently a Ph.D. student in Xi’an Jiaotong University. His research interests mainly focus on application of molecular ferroelectrics in photocatalytic water splitting for hydrogen evolution.

Huaiyu Lu

Huaiyu Lu obtained her master’s degree from Xi’an Jiaotong University. She is currently an engineer at BYD Company Limited.

Cheng Cheng

Cheng Cheng is an Associate Professor and Master’s Supervisor at the School of Chemical Engineering and Technology, Xi'an Jiaotong University (XJTU). He received his Ph.D. in Power Engineering and Engineering Thermophysics from XJTU in 2021. Dr. Cheng was selected for the XJTU Young Outstanding Talent Support Program. His primary research interests include solar-driven photothermal catalysis for hydrogen and hydrocarbon fuel production, and the synthesis and application of Covalent Organic Frameworks (COFs). He has led several projects, including those funded by the National Natural Science Foundation of China (NSFC) and a sub-project of the National Key Research and Development Program of China. He has published over 20 SCI-indexed papers with an H-index of 26.

Wengao Zeng

Wengao Zeng received his Ph.D. in Power Engineering and Engineering Thermal Physics of Xi’an Jiaotong University. His research interests focus on photocatalytic water splitting.

Xiangjiu Guan

Xiangjiu Guan Xiangjiu Guan obtained his PhD degree in Power Engineering and Engineering Thermaldynamics under the supervision of Prof. Liejin Guo from Xi’an Jiaotong University in 2018. During 2015–2016, he was a joint PhD student in the Department of Electrical and Computing Engineering at McGill University under the supervision of Prof. Zetian Mi. He is currently Associate Professor in the State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University. His research interests focus on catalysts and devices for solar-to-fuel conversion.

Liuhao Mao

Liuhao Mao received his Ph.D. in Power Engineering and Engineering Thermal Physics of Xi’an Jiaotong University. His research interests focus on hydrothermal synthesis of materials in supercritical fluids.

Li Tian

Li Tian received his Ph.D. in Power Engineering and Engineering Thermal Physics of Xi’an Jiaotong University. His research realm was photoelectrochemical water splitting for hydrogen.

Jinwen Shi

Jinwen Shi Dr. Jinwen Shi is a professor in the School of Energy and Power Engineering, Xi’an Jiaotong University. He received his Ph.D. of Power Engineering and Engineering Thermophysics under the supervision of Prof. Liejin Guo at Xi’an Jiaotong University in 2012. He worked as a visiting Ph.D. student (2008–2009) under the supervision of Prof. Jinhua Ye at National Institute for Materials Science in Japan. His research interests focus on solar-driven hydrogen and hydrocarbon fuel production, solar-driven atmospheric water harvesting and hydrogen production, and supercritical-fluid based photothermal catalysis. He is among the Stanford University’s Top 2% Scientists list (2023–2025).

Liejin Guo

Liejin Guo has been elected as a member of the Chinese Academy of Sciences (2017) and a fellow of The World Academy of Sciences (2021)，and is an scientist of engineering thermophysics and energy utilization, mainly focusing on the research on energy power multiphase flow and hydrogen energy science and technology. He is currently a professor and doctoral advisor of Xi’an Jiaotong University, the director of the State Key Laboratory of Multiphase Flow in Power Engineering, the founding director of the International Research Center for Renewable Energy, the founder and academic leader of the Department of New Energy Science and Engineering of Xi’an Jiaotong University, and the director of the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China. He is the deputy editor in Chief of Journal of Engineering Thermophysics. He is also a member of the editorial board and advisory board of journals such as International Journal of Hydrogen Energy, International Journal of Multiphase Flow, International Journal of Heat and Mass Transfer, and eScience. He has been serving as member of Scientific Committee of the International Centre for Heat and Mass Transfer (ICHMT), Corresponding member of the International Information Center for Multiphase Flow (ICEM), and member of the International Association for Hydrogen Energy (IAHE). As the first author, he won 2 second prizes in National Natural Science and 1 second prize in National Technical Invention.

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Abstract

As one of the most promising metal-free photocatalysts for renewable H₂ evolution, graphitic carbon nitride (g-C₃N₄) has attracted notable attention. Regulating its morphology and electronic structure is crucial for enhancing its performance. In this work, aromatic small molecules and melamine were hydrothermally cotreated to form a novel supramolecular precursor, which was subsequently calcined to obtain a π–π conjugated structure of g-C₃N₄ photocatalyst. The introduction of benzene-ring structures expanded the conjugated system and promoted the excitation of π electrons, thereby broadening the light-absorption range of g-C₃N₄. The synergism of bromine and chlorine provided abundant active sites for g-C₃N₄, greatly promoted the migration of photogenerated charge carriers, and reduced the recombination probability, thus improving in photocatalytic performance. Therefore, the g-C₃N₄ photocatalyst obtained from 2-bromo-5-chlorobenzoic acid-derived supramolecular precursor exhibited a visible-light (λ ≥ 400 nm) photocatalytic H₂ evolution activity of 839.8 μmol/(h g), which was about three times that of the unmodified g-C₃N₄. This work offers a novel perspective for g-C₃N₄ application in the field of photocatalysis and expands the utilization of aromatic small molecules in photocatalysts modification.

Keywords

Copolymerization / Graphitic carbon nitride / Hydrogen / Photocatalysis / Solar energy

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Chongze Cai, Huaiyu Lu, Cheng Cheng, Wengao Zeng, Xiangjiu Guan, Liuhao Mao, Li Tian, Jinwen Shi, Liejin Guo. Aromatic Ring-Coordinated g-C₃N₄ Nanotubes for Enhanced Photocatalytic H₂ Evolution. Transactions of Tianjin University, 2025, 31(6): 555-566 DOI:10.1007/s12209-025-00454-0

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