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Covalent triazine frameworks with Ru molecular catalyst for efficient photocatalytic oxygen evolution reaction

共价三嗪框架负载钌分子催化剂用于高效光催化析氧反应

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Abstract

The development of efficient oxygen evolution reaction (OER) photocatalysts to enable solar-driven photocatalytic water splitting into oxygen has been tremendously challenging, primarily due to the low oxygen evolution efficiency caused by intrinsically sluggish kinetics. Herein, we report the design of a novel “host-guest” photocatalytic system that incorporates the molecular ruthenium (Ru) catalyst into covalent triazine framework (CTF) channels through a facile immersion treatment. The CTF acts as the photosensitizer and support material, while the mononuclear Ru-based complex Ru-bda-Isoq acts as a molecular water-oxidation catalyst. Remarkably, Ru-bda-Isoq@CTF-Bph achieves an excellent oxygen evolution rate of up to 2308 µmol g−1 h−1 under visible light irradiation for 5 h. The structural matching between the porous photosensitizer and molecular catalyst is found to play a very critical role in achieving the high performance, and the specificity and universality of this system are also highlighted. This strategy provides valuable insights into the design of efficient water oxidation photocatalytic systems.

摘要

由于析氧反应的内在动力学缓慢, 开发高效的光催化析氧反应催化剂, 以利用太阳能进行光催化分解水产氧, 面临着巨大的挑战. 本研究设计了一种新型的“主-客体”光催化系统, 通过简单的预负载将单位点钌(Ru)分子催化剂引入共价三嗪框架(CTFs)的孔道内. 其中, CTFs作为光敏剂和光催化载体, 单核钌配合物Ru-bda-Isoq作为分子水氧化催化剂. 在可见光照射下, Ru-bda-Isoq@CTF-Bph 在5 h内平均析氧速率达到2308 µmol g−1 h−1, 其性能超过了大多数有机光催化剂. 同时, 研究还发现多孔光敏剂与分子催化剂之间的结构匹配起着非常关键的作用. 该体系具有广泛的适用性, 这一策略有助于高效水氧化光催化系统的设计.

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Acknowledgements

The authors thank the Analysis and Testing Center, Huazhong University of Science and Technology for the assistance in the characterization of materials. This work was financially supported by the National Natural Science Foundation of China (22161142005 and 21975086), and the Science and Technology Department of Hubei Province (2019CFA008).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China

    Ruixue Sun  (孙瑞雪), Xunliang Hu  (胡勋亮), Chang Shu  (舒畅), Yantong Guo  (郭彦彤), Xiaoyan Wang  (王笑颜) & Bien Tan  (谭必恩)

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  1. Ruixue Sun  (孙瑞雪)
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  2. Xunliang Hu  (胡勋亮)
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  3. Chang Shu  (舒畅)
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  4. Yantong Guo  (郭彦彤)
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  5. Xiaoyan Wang  (王笑颜)
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  6. Bien Tan  (谭必恩)
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Contributions

Author contributions Tan B and Hu X conceived the project and designed the experiments. Sun R performed the experiments and analyzed the data. Sun R, Hu X, Wang X and Tan B co-wrote the manuscript. Shu C and Guo Y helped in collecting the optical and electronic data.

Corresponding author

Correspondence to Bien Tan  (谭必恩).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Supplementary information Experimental details and supporting data are available in the online version of the paper.

Bien Tan is a professor at the School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology (HUST). He received his PhD degree in 1999 from the College of Materials at South China University of Technology. He then joined Beijing Institute of Aeronautical Materials for postdoctoral research at the National Laboratory of Advanced Composites (1999–2001). He worked as a post-doc research associate at the University of Liverpool (2001–2007). He then returned to China and joined HUST in September 2007 as a professor. His main research interests include polymeric materials, microporous materials, hydrogen storage, metal nano-particles, and high throughput materials methodology.

Ruixue Sun received her Bachelor’s degree in materials chemistry from Ludong University in 2016. She then received her Master’s degree in materials physics and chemistry from Shandong University in 2019. She is currently studying for her PhD degree in the group of Professor Bien Tan in polymer chemistry and physics at HUST. Her current research interests focus on the synthesis and applications of covalent triazine frameworks.

Xunliang Hu received his Bachelor’s degree in applied chemistry from Huazhong Agricultural University in 2013. He then received his Master’s degree in chemical engineering from Hubei University of Technology in 2017. He then received PhD degree in materials chemistry from HUST in 2022. His current research interests focus on the synthesis and applications of covalent triazine frameworks.

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Sun, R., Hu, X., Shu, C. et al. Covalent triazine frameworks with Ru molecular catalyst for efficient photocatalytic oxygen evolution reaction. Sci. China Mater. 67, 642–649 (2024). https://doi.org/10.1007/s40843-023-2714-x

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