Homogeneous catalysts are widely used in the chemical industry. Compared to their heterogeneous counterparts, homogeneous catalysts exhibit not only higher reactivity, but also well-defined active sites convenient for mechanistic study and structural design. However, the difficulty in recycling and removal of homogeneous catalysts after use increases production cost and also raises safety and environmental concerns. Therefore, the immobilization of homogeneous catalysts within a pore carrier can maximize their application potential.<br/><br/>Metal-organic frameworks (MOFs) are an excellent class of porous materials for hosting homogeneous catalyst because their tunable pores can be customized to meet the size, shape and functionality of the guests. However, the dilemma is that the aperture size of the MOF must be larger than the catalyst to enable the encapsulation process, in which case catalyst leaching is inevitable.<br/><br/>Confronting this challenge, this talk presents two strategies to immobilize homogeneous catalysts in large aperture MOFs. The first strategy utilizes a surface-focused polymerization reaction to rapidly deposit a sub-10 nm uniform polymer layer on the MOF surface to seal the homogeneous catalyst in the pore whereas the second strategy takes advantage of pore partitioning to devide MOF pores into smaller segments, thus preventing the leaching of the catalyst. The obtained "heterogenized" homogeneous catalysts can be easily recycled many times for pollutant decomposition and other catalytic reactions.

Surface-seal and pore partitioning for the immobilization of homogeneous catalysts within metal-organic frameworks for pollutant removal

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ACS Fall 2022

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