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In situ meso-tetra (4-carboxyphenyl) porphyrin ligand substitution in Hf-MOF for enhanced catalytic activity and stability in photoredox reactions

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Abstract

Though there are numerous intrinsic merits of metal-organic frameworks (MOFs), low charge separation efficiency has imposed heavy restrictions on their photocatalytic application. Herein, in situ porphyrin ligand substitution, as a strategy for improving the charge separation efficiency and increasing the amounts of active sites, has been designed and realized in a Hf-biphenyl dicarboxylic acid (BPDC) MOF. Specifically, a size and geometry matched meso-tetra (4-carboxyphenyl) porphyrin (TCPP) ligand was selected and doped into Hf-BPDC MOF by forming coordinating bonds with Hf centers, forming dual-ligand Hf-BPDC-TCPP MOF. The resultant Hf-BPDC-TCPP MOF showed significantly improved activity and chemical stability in the photocatalytic H2 generation (261 μmol·g−1·h−1) and tetracycline (TC) degradation reactions (95.8%), which was 48 and 1.47 folds higher than that of the Hf-BPDC MOF. Photophysical and electrochemical studies revealed that the introduction of porphyrin ligand could generate a stronger internal electric field for boosting the charge separation and transfer, increase the specific surface area for providing more active sites, and narrow the band gap to enhance the visible light absorption. This in situ ligand substitution method provides a promising approach to build a tunable platform for constructing high-performance MOF photocatalysts.

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摘要

标题：Meso-四（4-羧基苯基）卟啉配体原位取代提高Hf-MOF在光催化氧化还原反应中活性和稳定性 作者：胡杰、劳红新、许修武、王伟康、王乐乐、刘芹芹 单位：江苏大学材料科学与工程学院，江苏镇江212013 摘要：尽管金属有机骨架(MOFs)具有许多内在优点，但较低的电荷分离效率严重制约了其光催化应用。本文通过配体原位取代策略提高了Hf-联苯二甲酸基MOF材料的电荷分离效率并增加了活性位点。具体而言，选择尺寸和几何形状匹配的中四(4-羧基苯基)卟啉(TCPP)配体，通过与Hf中心形成配位键，将其掺杂到Hf-BPDC-TCPP MOF中，形成双配体Hf-BPDC-TCPP MOF。制备的Hf-BPDC-TCPP MOF在光催化产H2 (261 μmol g-1 h-1)和四环素(TC)降解反应(95.8%)中的性能和化学稳定性显著提高，分别达到单配体Hf-BPDC MOF的48和1.47倍。光物理和电化学测试结果表明，卟啉配体的引入可以产生更强的内部电场，促进电荷的分离和转移，增加比表面积，提供更多的活性位点，窄化带隙，增强可见光吸收。这种原位配体取代方法为构建高性能MOF光催化剂提供了一种有前途的可调平台。

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Acknowledgements

This work was financially supported by the National Nature Science Foundation of China (Nos. 22102064 and 21972058). Dr. L.W. was supported by the Open Project Program of Fujian Provincial Key Laboratory of Ecology-Toxicological Effects and Control for Emerging Contaminants, Putian University.

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  1. School of Materials Science and Engineering, Jiangsu University, Zhenjiang, 212013, China

    Jie Hu, Hong-Xin Lao, Xiu-Wu Xu, Wei-Kang Wang, Le-Le Wang & Qin-Qin Liu

  2. Fujian Provincial Key Laboratory of Ecology-Toxicological Effects and Control for Emerging Contaminants, Putian University, Putian, 351100, China

    Le-Le Wang

  3. College of Chemistry and Materials, Engineering Research Center of Carbon Neutrality, Anhui Normal University, Wuhu, 241002, China

    Wei-Kang Wang

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Hu, J., Lao, HX., Xu, XW. et al. In situ meso-tetra (4-carboxyphenyl) porphyrin ligand substitution in Hf-MOF for enhanced catalytic activity and stability in photoredox reactions. Rare Met. 43, 2682–2694 (2024). https://doi.org/10.1007/s12598-023-02595-4

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