Metal−organic frameworks (MOFs) are an emerging class of porous materials constructed from metal-containing nodes and organic linkers. Due to their structural and functional tunability as well as their ever-expanding application scope, MOFs have become one of the most fascinating class of materials for both scientists and engineers. The unprecedented level of structural control at molecular precision has brought new opportunities to heterogeneous catalysis. Despite numerous advantages, the applications of MOFs in catalysis are ultimately limited by their stability under harsh conditions. Therefore, we have been focusing on the development of stable MOFs based on trivalent and tetravalent metals (M (III) and M (IV)), which tend to possess much greater stability due to the increased strength and kinetic inertness of the metal-carboxylate bonds. However, the inert metal-carboxylate bond has posed challenges for the synthesis and pore engineering of stable MOFs for catalysis. The conventional “one-pot” synthetic method lacks control over the reaction pathways and the products, which essentially limits the construction of robust MOF-catalysts. By judicious kinetic control, we have developed multiple synthetic strategies, which have led to the “total synthesis” approach, through which a target MOF can be retro-synthetically designed and synthesized. A series of synthetic strategies have been developed to functionalize stable MOFs by “layer-on” molecular elaborations to preformed coordination assemblies, which together form a synthetic toolbox. “Total synthesis” multi-component MOFs was realized by sequentially applying the above mentioned synthetic methods under kinetic considerations. These MOFs with high stability and precisely controlled pore environments are critical for a variety of applications such as cooperative catalysis.

Precise pore engineering of stable metal−organic frameworks for heterogeneous catalysis

256th National Meeting (2018)

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