Transformation of Type III to Type II Porous Liquids by Tuning Surface Rigidity of Rhodium(II)‐Based Metal‐Organic Polyhedra for CO2 Cycloaddition

Porous liquids (PLs), a summation of porous hosts and bulky solvents bestowing permanent cavities, are the prominent emerging materials. Despite great efforts, exploration of porous hosts and bulky solvents is still needed to develop new PL systems. Metal‐organic polyhedra (MOPs) with discrete molec...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2023-08, Vol.62 (31), p.e202306495-n/a
Main Authors: Dinker, Manish Kumar, Li, Meng‐Meng, Zhao, Kan, Zuo, Mingrui, Ding, Lifeng, Liu, Xiao‐Qin, Sun, Lin‐Bing
Format: Article
Language:English
Subjects:
Carbon dioxide
Catalytic activity
CO2 Adsorption
Cycloaddition
Ionic Liquid
Ionic liquids
Metal-Organic Polyhedra
Molecular structure
Polyhedra
Porous Liquid
Rhodium
Rigidity
Solubilization
Solvents
Tuning
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Summary:Porous liquids (PLs), a summation of porous hosts and bulky solvents bestowing permanent cavities, are the prominent emerging materials. Despite great efforts, exploration of porous hosts and bulky solvents is still needed to develop new PL systems. Metal‐organic polyhedra (MOPs) with discrete molecular architectures can be considered as porous hosts; however, many of them are insoluble entities. Here we report the transformation of type III PL to type II PLs by tuning the surface rigidity of insoluble MOP, Rh24L24, in a bulky ionic liquid (IL). Functionalization of N‐donor molecules on Rh−Rh axial sites ensue their solubilization in bulky IL which confer type II PLs. Experimental and theoretical studies reveal the bulkiness of IL as per the cage apertures, and the cause of their dissolution as well. The obtained PLs, capturing more CO2 than neat solvent, have depicted higher catalytic activity for CO2 cycloaddition compared to individual MOPs and IL. By incorporating N‐donor molecules on the Rh−Rh axial sites of insoluble RhMOP, and making it soluble as porous host in bulky ionic liquid, a type III porous liquid was transformed into type II porous liquids for better catalyzing the cycloaddition of CO2.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202306495