<br>具有大纳米孔结构的纤维状 Zr-MOF 纳米酶气凝胶用于增强有机磷毒素的催化水解,Advanced Materials

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具有大纳米孔结构的纤维状 Zr-MOF 纳米酶气凝胶用于增强有机磷毒素的催化水解
Advanced Materials ( IF 27.4 ) Pub Date : 2023-06-13 , DOI: 10.1002/adma.202300951
Kaikai Ma _{1,

2} , Yuk Ha Cheung ₂ , Kent O Kirlikovali ₁ , Haomiao Xie ₁ , Karam B Idrees ₁ , Xiaoliang Wang ₁ , Timur Islamoglu ₁ , John H Xin ₂ , Omar K Farha _{1,

3}

Affiliation

具有路易斯酸催化位点的金属有机框架（MOF），例如锆基 MOF（Zr-MOF），包含一类不断增长的磷酸酶样纳米酶，可以降解有毒的有机磷酸酯农药和神经毒剂。将 MOFs 从合成粉末合理地设计和成型为分层多孔整体材料对于其在新兴应用中的使用至关重要，例如用于空气和水净化的过滤器以及个人防护装备。然而，一些挑战仍然限制了实际 MOF 复合材料的生产，包括需要复杂的反应条件、所得复合材料中 MOF 催化剂负载量低以及基于 MOF 的活性位点的可及性较差。为了克服这些限制，开发了一种快速合成方法，将 Zr-MOF 纳米酶涂层引入纤维素纳米纤维中，从而形成具有高 MOF 负载量的可加工整体气凝胶复合材料。这些复合材料的结构中嵌入了 Zr-MOF 纳米酶，分级的宏观-微观孔隙度使得催化活性位点具有良好的可及性。这种多方面的合理设计策略，包括选择具有多个催化位点的MOF、微调涂层形态以及制造分层结构的整体气凝胶，为有机磷基神经毒剂模拟物的高效连续水解解毒提供了协同效应以及来自受污染水中的杀虫剂。

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Fibrous Zr-MOF Nanozyme Aerogels with Macro-Nanoporous Structure for Enhanced Catalytic Hydrolysis of Organophosphate Toxins

Metal–organic frameworks (MOFs) with Lewis acid catalytic sites, such as zirconium-based MOFs (Zr-MOFs), comprise a growing class of phosphatase-like nanozymes that can degrade toxic organophosphate pesticides and nerve agents. Rationally engineering and shaping MOFs from as-synthesized powders into hierarchically porous monoliths is essential for their use in emerging applications, such as filters for air and water purification and personal protection gear. However, several challenges still limit the production of practical MOF composites, including the need for sophisticated reaction conditions, low MOF catalyst loadings in the resulting composites, and poor accessibility to MOF-based active sites. To overcome these limitations, a rapid synthesis method is developed to introduce Zr-MOF nanozyme coating into cellulose nanofibers, resulting in the formation of processable monolithic aerogel composites with high MOF loadings. These composites contain Zr-MOF nanozymes embedded in the structure, and hierarchical macro-micro porosity enables excellent accessibility to catalytic active sites. This multifaceted rational design strategy, including the selection of a MOF with many catalytic sites, fine-tuning the coating morphology, and the fabrication of a hierarchically structured monolithic aerogel, renders synergistic effects toward the efficient continuous hydrolytic detoxification of organophosphorus-based nerve agent simulants and pesticides from contaminated water.

更新日期：2023-06-13

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