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An Efficient Synthesis Strategy for Metal-Organic Frameworks: Dry-Gel Synthesis of MOF-74 Framework with High Yield and Improved Performance

机译:金属-有机骨架的有效合成策略:高产率和改进性能的干凝胶合成MOF-74骨架

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摘要

Vapor-assisted dry-gel synthesis of the metal-organic framework-74 (MOF-74) structure, specifically Ni-MOF-74 produced from synthetic precursors using an organic-water hybrid solvent system, showed a very high yield (>90% with respect to 2,5-dihydroxyterepthalic acid) and enhanced performance. The Ni-MOF-74 obtained showed improved sorption characteristics towards CO2 and the refrigerant fluorocarbon dichlorodifluoromethane. Unlike conventional synthesis, which takes 72 hours using the tetrahydrofuran-water system, this kinetic study showed that Ni-MOF-74 forms within 12 hours under dry-gel conditions with similar performance characteristics, and exhibits its best performance characteristics even after 24 hours of heating. In the dry-gel conversion method, the physical separation of the solvent and precursor mixture allows for recycling of the solvent. We demonstrated efficient solvent recycling (up to three times) that resulted in significant cost benefits. The scaled-up manufacturing cost of Ni-MOF-74 synthesized via our dry-gel method is 45% of conventional synthesis cost. Thus, for bulk production of the MOFs, the proposed vapor-assisted, dry-gel method is efficient, simple, and inexpensive when compared to the conventional synthesis method.
机译:金属有机框架74(MOF-74)结构的蒸汽辅助干凝胶合成,特别是使用有机-水混合溶剂系统由合成前体生产的Ni-MOF-74,具有很高的收率(> 90% (相对于2,5-二羟基对苯二甲酸)和更高的性能。所获得的Ni-MOF-74对CO 2和制冷剂碳氟化合物二氯二氟甲烷显示出改善的吸附特性。与使用四氢呋喃-水系统进行常规合成需要72个小时的时间不同,该动力学研究表明Ni-MOF-74在干凝胶条件下在12个小时内会形成,具有相似的性能特征,即使经过24个小时的反应仍显示出最佳的性能特征。加热。在干凝胶转化方法中,溶剂和前体混合物的物理分离允许溶剂的再循环。我们展示了有效的溶剂回收(多达三遍),从而带来了可观的成本优势。通过我们的干凝胶法合成的Ni-MOF-74的放大制造成本为传统合成成本的45%。因此,对于MOF的批量生产,与常规合成方法相比,所提出的蒸气辅助干凝胶法是有效,简单且廉价的。

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