近红外响应光热催化降解有机污染物的多金属酸氧基配位聚合物结构设计

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Molecular Structure Pub Date : 2025-10-09 DOI:10.1016/j.molstruc.2025.144302

Wenxu Ma, Yunqiong Yang

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引用次数: 0

摘要

采用水热法合成了[Cu3(biim)6(PMo12O40)]·5H2O （jo -46）和[Cu2(Cl)(impy)4][PMo12O40]·H2O （jo -47）两种新型多金属氧酸盐配位聚合物（POM@CPs）（biim = 2,2′-双咪唑，impy = 2-（咪唑-2-基）吡啶）。单晶x射线衍射显示，joo -46形成了由氢键连接的阶梯型链构成的三维（3D）超分子结构，而joo -47则呈现出由Cu-impy片段和[PMo12O40]3−团簇组成的三维超分子结构。这些材料具有广泛的吸收范围和优异的光热转换效率，大大提高了光催化性能和太阳能利用率。在模拟阳光照射下，joo -47的表面温度在120s内由32℃升高到166℃。与j -46相比，j -47具有更宽的光吸收范围和更高的光热转换效率（44.4% vs. 29.1%）。在joo -47/H2O2体系中，95.2%的盐酸四环素在50 min内被降解，速率常数为0.06 min−1。此外，该系统还能有效去除各种有机污染物。这项工作为设计高效的POM@CP-based光热水净化催化剂提供了见解。

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Structural design of polyoxometalate-based coordination polymers for near-infrared-responsive photothermal catalytic degradation of organic pollutants

Two new polyoxometalate-based coordination polymers (POM@CPs), namely [Cu₃(biim)₆(PMo₁₂O₄₀)]·5H₂O (JOU-46) and [Cu₂(Cl)(impy)₄][PMo₁₂O₄₀]·H₂O (JOU-47), were synthesized via a hydrothermal method (biim = 2,2’-biimidazole, impy = 2-(imidazol-2-yl) pyridine). Single-crystal X-ray diffraction revealed that JOU-46 forms a three-dimensional (3D) supramolecular framework constructed from ladder-type chains linked by hydrogen bonds, whereas JOU-47 exhibits a 3D supramolecular architecture assembled from Cu-impy fragments and [PMo₁₂O₄₀]³⁻ clusters. Benefiting from their broad absorption range and excellent photothermal conversion efficiency, these materials significantly enhance photocatalytic performance and solar energy utilization. Under the irradiation of simulated sunlight, surface temperature of JOU-47 increased from 32 °C to 166 °C within 120 s. Compared with JOU-46, JOU-47 exhibited a broader light absorption range and a higher photothermal conversion efficiency (44.4% vs. 29.1%). In JOU-47/H₂O₂ system, 95.2% of tetracycline hydrochloride was degraded within 50 min, giving a rate constant of 0.06 min⁻¹. Moreover, this system can also efficiently remove various organic pollutants. This work provides insights for designing efficient POM@CP-based photothermal catalysts for water purification.

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来源期刊

Journal of Molecular Structure 化学-物理化学

CiteScore

7.10

自引率

15.80%

发文量

2384

审稿时长

45 days

期刊介绍： The Journal of Molecular Structure is dedicated to the publication of full-length articles and review papers, providing important new structural information on all types of chemical species including: • Stable and unstable molecules in all types of environments (vapour, molecular beam, liquid, solution, liquid crystal, solid state, matrix-isolated, surface-absorbed etc.) • Chemical intermediates • Molecules in excited states • Biological molecules • Polymers. The methods used may include any combination of spectroscopic and non-spectroscopic techniques, for example: • Infrared spectroscopy (mid, far, near) • Raman spectroscopy and non-linear Raman methods (CARS, etc.) • Electronic absorption spectroscopy • Optical rotatory dispersion and circular dichroism • Fluorescence and phosphorescence techniques • Electron spectroscopies (PES, XPS), EXAFS, etc. • Microwave spectroscopy • Electron diffraction • NMR and ESR spectroscopies • Mössbauer spectroscopy • X-ray crystallography • Charge Density Analyses • Computational Studies (supplementing experimental methods) We encourage publications combining theoretical and experimental approaches. The structural insights gained by the studies should be correlated with the properties, activity and/ or reactivity of the molecule under investigation and the relevance of this molecule and its implications should be discussed.