Generalized Approach for Rapid Aqueous MOF Synthesis by Controlling Solution pH,Crystal Growth & Design

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Generalized Approach for Rapid Aqueous MOF Synthesis by Controlling Solution pH
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2020-09-01 , DOI: 10.1021/acs.cgd.0c00895
Luke Huelsenbeck ₁ , Hongxi Luo ₁ , Prince Verma ₁ , Jillian Dane ₁ , Rachel Ho ₁ , Emily Beyer ₁ , Hailey Hall ₁ , Geoffrey M. Geise ₁ , Gaurav Giri ₁

Affiliation

Metal–organic frameworks (MOFs) are a promising class of functional materials with applications in catalysis, separations, electronics, and drug delivery, among others. Despite a range of techniques utilized for MOF synthesis, a generalizable and scalable approach has yet to be developed for producing MOFs without using environmentally damaging organic solvents. Here, we look at MOF synthesis as a reaction in an aqueous medium and propose new methods of measuring conversion and selectivity. We show that controlling reactant speciation via pH is a generalizable approach to producing the prototypical MOFs UiO-66, UiO-66-NH₂, ZIF-L, and HKUST-1 with space–time yields (STY) of over 2250 kg m^–3 day^–1, which is a 1 order of magnitude improvement for zirconium-based MOFs. We show that UiO-66-NH₂ crystallization is complete in 5 min at room temperature, with 70% of the extent of reaction completed by 30 s. Finally, we apply the rapid synthesis approach to coating cotton fabric with up to 20 wt % UiO-66-NH₂ using a sequential dip-coating (SQD) technique and demonstrate particulate matter (PM_1–4) filtration up to 85%. This work shows a green-chemistry-based, generalizable pathway to rapid synthesis for multiple MOFs and demonstrates its utility for filtration applications. The ability to produce alternative filtration materials is especially relevant under pandemic conditions, where SQD offers a rapid and high-throughput manner of providing air filtration by modifying commonly available textile materials.

中文翻译：

通过控制溶液pH值快速合成MOF的通用方法

金属有机框架（MOF）是一类很有前途的功能材料，其应用包括催化，分离，电子和药物传递等。尽管用于MOF合成的技术范围很广，但尚未开发出可通用且可扩展的方法来生产MOF，而不使用对环境有害的有机溶剂。在这里，我们将MOF合成视为在水性介质中的反应，并提出了测量转化率和选择性的新方法。我们表明，通过pH控制反应物的形态是生产原型MOF UiO-66，UiO-66-NH ₂，ZIF-L和HKUST-1的通用方法，时空产率（STY）超过2250 kg m ^{– 3}天^–1，这是基于锆的MOF的1个数量级的改进。我们显示UiO-66-NH ₂结晶在室温下5分钟内完成，其中70％的反应程度在30 s内完成。最后，我们应用快速合成方法，采用顺序浸涂（SQD）技术，以高达20 wt％的UiO-66-NH ₂涂层棉织物，并证明了颗粒物（PM _1-4）过滤率最高可达85％。这项工作显示了一种基于绿色化学的可通用途径，可以快速合成多个MOF，并证明了其在过滤应用中的实用性。在大流行条件下，生产替代性过滤材料的能力尤其重要，在SQD中，SQD通过修改常用的纺织材料提供了一种快速，高通量的空气过滤方法。

更新日期：2020-10-07

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