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Organic microstructure-induced hierarchically porous g-C3N4 photocatalyst

有机微结构诱导的分级多孔g-C3N4光催化剂

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Abstract

It is necessary to construct hierarchically porous photocatalysts to ensure high light absorption and electrochemical kinetics in photocatalysis. Carbon nitride (g-C3N4) appears to be a favorable choice, especially the tunable hollow micro/nanostructure. However, the facile preparation of g-C3N4 with hierarchical pores still faces challenge. Here, we firstly report a facile preparation of hierarchically porous g-C3N4 with uniform organic microstructure as a soft template. The template is in situ formed in thiourea precursor solution, and its similar π-conjugated structure to g-C3N4 makes it effective in modifying the condensation of g-C3N4. The layer thickness of the as-prepared g-C3N4 is about 3–4 nm. And the resultant g-C3N4 possesses hierarchical meso/macropores with a specific surface area of 27.34 m2 g−1 and pore volume of 0.18 cm3 g−1, approximately 6.2 and 9.0 times, respectively, higher than that of the unmodified one. This favors the charge/mass transport process, hence rendering the catalyst a 2.4-fold enhancement in photodegrading organic pollutant with H+ and ·O −2 as the predominant species. At the same time, the photostability can be guaranteed with only 20% loss of its efficiency after long-term use.

摘要

为了保证光催化的高光吸收和电化学动力学, 构建分级多孔光 催化剂十分必要. 类石墨相氮化碳(g-C3N4)易于合成、理化性质稳定、 稳定性好和带隙合适等优点, 特别是其可调的微/纳米结构, 使其成为 分级多孔光催化剂一个很好的选择. 然而, 具有层次孔的g-C3N4的简易 制备仍然是一个难点. 本文中, 我们首次用均匀的有机微结构作为软模 板, 用简单方法制备了分级多孔g-C3N4. 该有机微纳结构模板是在硫脲 前驱体溶液中原位形成的, 与g-C3N4相似的π共轭结构使其能够有效修 饰g-C3N4的分子结构. 结果表明, 合成的g-C3N4具有分级的中孔和大孔, 比表面积为27.34 m2 g−1, 孔体积为0.18 cm3 g−1, 分别是未改性g-C3N4的 6.2倍和9.0倍. 这种分级多孔结构有利于电荷/质量传输过程, 使其光降 解有机污染物能力增强了2.4倍. 同时, 此光催化剂具有良好的光稳定 性, 长期使用100分钟后效率仅损失20%.

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Acknowledgements

This work was financially supported by the National Key R&D Program of China (2021YFB3802200) and the Scientific and Technological Innovation Foundation of Shunde Graduate School, University of Science and Technology Beijing (BK19AE027 and BK20BE022).

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Authors and Affiliations

  1. School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083, China

    Jiaqi Dong  (董嘉祺), Zhengqi Gong  (巩正奇), Yingzhi Chen  (陈颖芝), Jiaxin Li  (李家馨), Rongsheng Deng  (邓荣胜) & Lu-Ning Wang  (王鲁宁)

  2. Shunde Graduate School of University of Science and Technology Beijing, Foshan, 528399, China

    Yingzhi Chen  (陈颖芝), Wenjie Zhou  (周文杰), Mingqiang Yang  (杨明强) & Lu-Ning Wang  (王鲁宁)

  3. School of Chemistry and Chemical Engineering, Mudanjiang Normal University, Mudanjiang, 157011, China

    Guodong Hao  (郝国栋)

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  1. Jiaqi Dong  (董嘉祺)
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Contributions

Gong Z performed the experiments with support from Dong J; Zhou W draw part of illustrations. Chen Y conceived the work and wrote the paper. All authors contributed to the general discussion.

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Correspondence to Yingzhi Chen  (陈颖芝), Guodong Hao  (郝国栋) or Lu-Ning Wang  (王鲁宁).

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The authors declare that they have no conflict of interest.

Yingzhi Chen is an associate professor at the School of Materials Science and Engineering, University of Science and Technology Beijing. She received her PhD degree in chemistry from the Institute of Technical Institute of Physics & Chemistry, Chinese Academy of Sciences in 2012 after she got her MS degree in chemistry from Beijing Normal University. Her current research focuses on the design and synthesis of novel organic semiconductor nanocrystals and their applications in photocatalysis and biosensing.

Lu-Ning Wang is a professor at the School of Materials Science and Engineering, University of Science and Technology Beijing. He received his BE and MS degrees in materials science and engineering from the University of Science and Technology Beijing in 2002 and Tsinghua University in 2005, respectively. He received another ME and PhD degrees in medical science and biomedical engineering from the University of Alberta in 2007 and 2011, respectively. His research interests include optoelectronic materials and biodgradable materials.

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Dong, J., Gong, Z., Chen, Y. et al. Organic microstructure-induced hierarchically porous g-C3N4 photocatalyst. Sci. China Mater. 66, 3176–3188 (2023). https://doi.org/10.1007/s40843-022-2463-8

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