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Harnessing Bottom-up Self-Assembly to Position Five Distinct Components in an Ordered Porous Framework.

Angewandte Chemie 2019 Februrary 19
Positioning a diverse set of building blocks in a well-defined array allows for cooperativity amongst them and the systematic programming of functional properties. Extending this concept to porous metal-organic frameworks (MOFs) is challenging since installing multiple components in a well-ordered framework requires careful design of the lattice topology, judicious selection of building blocks, and precise control of the crystallization parameters. In this work, we report how we have met these challenges to prepare the first quinary MOF structure, FDM-8, by bottom-up self-assembly. FDM-8 is constructed from two metals, Zn(II) and Cu(I), and three distinct carboxylate- and pyrazolate-based linkers. By employing a strategy of deconstructing the nodes and edges in the network, FDM-8 equals the record for the highest number of well-ordered components in a crystalline molecular solid. With a surface area of 3643 m2 g-1, FDM-8 features hierarchical pores, which contribute to an outstanding methane storage capacity at high pressure. Furthermore, the FDM-8 structure evolves with application of reticular chemistry, whereby functional groups that are introduced to the linkers become compartmentalized in predetermined arrays in the framework pores. FDM-8 and its functional derivatives achieve a new level of MOF complexity and represents a further step towards the diversity seen in natural systems, which underlies their exquisite functionality.

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