具有 1,3,6,8-四（吡啶-4-基）芘的耐强碱锌有机骨架，用于高效光催化析氢,Journal of Materials Chemistry A

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具有 1,3,6,8-四（吡啶-4-基）芘的耐强碱锌有机骨架，用于高效光催化析氢
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2023-07-06 , DOI: 10.1039/d3ta02520a
Guo-Li Yang _{1,

2} , Yao Xie ₁ , Zhuo-Hao Jiao ₁ , Jian Zhao ₁ , Sheng-Li Hou ₁ , Ying Shi ₁ , Jie Han ₁ , Bin Zhao ₁

Affiliation

使用金属有机框架（MOF）的光催化析氢在缓解环境和能源危机方面具有巨大潜力。在此，基于1,3,6,8-四(吡啶-4-基)芘(TTPy)成功合成了三维锌有机骨架( 1 )。化合物1表现出良好的光吸收性，吸收限约为600 nm。重要的是，1在TEOA溶液中可以保持结晶状态，甚至在5 M NaOH水溶液中也能保持稳定，这表明1具有较高的耐碱性。光催化结果表明，1作为光催化剂，以TEOA为牺牲剂，具有较高的产H _{2活性，且H}即使在不添加光敏剂的长反应时间（35小时）下，_2的演化速率也为315.06 μmol g^-1 h^{-1 。}机理探索表明，平行配体之间的π-π相互作用、高碱稳定性和光吸收能力、良好的光电流响应以及化合物1合适的带隙是其高光催化活性的原因。密度泛函理论（DFT）计算进一步表明，实验能隙1与理论带隙非常一致。该工作为碱稳定MOFs在光催化领域的开发提供了新的策略。

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A strong-alkali resistant zinc–organic framework with 1,3,6,8-tetra(pyridin-4-yl)pyrene for efficient photocatalytic hydrogen evolution

Photocatalytic hydrogen evolution using metal–organic frameworks (MOFs) has tremendous potential for relieving the environmental and energy crises. Herein, a three dimensional zinc–organic framework (1) was successfully synthesized based on 1,3,6,8-tetra(pyridin-4-yl)pyrene (TTPy). Compound 1 exhibited a good light absorption with an absorption edge at approximately 600 nm. Importantly, 1 can maintain the crystalline state in TEOA solution, and even remain stable in a 5 M NaOH aqueous solution, suggesting 1 has high alkali resistance. Photocatalytic results indicate that 1 as a photocatalyst has high activity for H₂ production with TEOA as a sacrificial agent, and the H₂ evolution rate is 315.06 μmol g⁻¹ h⁻¹ even under long reaction time (35 h) without the addition of photosensitizers. Mechanism explorations suggest that the π–π interaction between parallel ligands, high alkali-stability and light-absorbing ability, good photocurrent response, and suitable band gap of compound 1 are responsible for the high photocatalytic activity. Density functional theory (DFT) calculations further reveal that the experimental energy gap of 1 is well consistent with the theoretical bandgap. This work provides a new strategy for the exploitation of alkali-stable MOFs in the photocatalysis field.

更新日期：2023-07-06

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