Green synthesis of Zr-based metal–organic framework hydrogel composites and their enhanced adsorptive properties,Inorganic Chemistry Frontiers

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Green synthesis of Zr-based metal–organic framework hydrogel composites and their enhanced adsorptive properties
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2020-09-25 , DOI: 10.1039/d0qi00840k
Shirell E Klein ₁ , Joshua D Sosa ₁ , Alexander C Castonguay ₂ , Willmer I Flores ₁ , Lauren D Zarzar _{2,

3,

4} , Yangyang Liu ₁

Affiliation

Metal–organic frameworks (MOFs) have emerged as promising candidates for a wide range of applications due to their high surface area and customizable structures, however, the minimal external hydrophilicity of MOFs has limited their biomedical implementations. Structuring of MOFs within polymer frameworks is an approach used to create hybrid materials that retain many of the MOF characteristics (e.g. high adsorption capacity) but expand the range of mechanical and surface properties as well as form factors accessible. Using this approach, hybridizing MOFs with hydrophilic hydrogels can give rise to materials with improved hydrophilicity and biocompatibility. Here, we describe the synthesis of the first Zr-based MOF-hydrogel hybrid material (composite 3) using a green chemistry approach, in which only water was used as the solvent and relatively low temperature (50 °C) was applied. Using methylene blue (MB) as a probe molecule, composite 3 exhibited greater adsorption capacity than the MOF or the hydrogel alone in aqueous solution at most tested pH values (all except pH 13). At an initial MB concentration of 0.0096 mg mL⁻¹ (30.014 μM) and neutral pH conditions, this new hybrid presented the highest loading of MB among similar materials (MB adsorbed = 4.361 ± 0.092 mg MB per g Zr, partition coefficient = 0.172 ± 0.004 mg g⁻¹ μM⁻¹) and largely retained its adsorption capacity under varied conditions (pH 1–13 and 0.2–1.0 M NaCl), rendering possible applications in drug delivery and the removal of tumor contrast agent/dye with minimal leakage due to its broad chemical stability.

中文翻译：

锆基金属有机骨架水凝胶复合材料的绿色合成及其增强的吸附性能

金属有机框架（MOF）由于其高表面积和可定制的结构而成为广泛应用的有希望的候选者，然而，MOF的最小外部亲水性限制了其生物医学应用。在聚合物框架内构建 MOF 是一种用于创建混合材料的方法，该材料保留了 MOF 的许多特性（例如高吸附能力），但扩大了机械和表面性能以及可用的形状因素的范围。使用这种方法，将 MOF 与亲水性水凝胶杂交可以产生具有改善的亲水性和生物相容性的材料。在这里，我们描述了使用绿色化学方法合成第一种基于Zr基MOF-水凝胶杂化材料（复合材料3 ），其中仅使用水作为溶剂并应用相对较低的温度（50°C）。使用亚甲基蓝（MB）作为探针分子，在大多数测试的pH值（除pH 13外）的水溶液中，复合材料3表现出比单独的MOF或水凝胶更大的吸附能力。在初始 MB 浓度为 0.0096 mg mL ⁻¹ (30.014 μM) 和中性 pH 条件下，这种新型混合材料在类似材料中呈现出最高的 MB 负载量（MB 吸附 = 4.361 ± 0.092 mg MB 每 g Zr，分配系数 = 0.172 ± 0.004 mg g ⁻¹ μM ⁻¹ ），并且在不同条件（pH 1-13和0.2-1.0 M NaCl）下很大程度上保留了其吸附能力，使得在药物输送和肿瘤造影剂/染料去除方面的应用成为可能，并且由于泄漏最小其广泛的化学稳定性。

更新日期：2020-11-12

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