- Title
- Ligand functionalization in zirconium-based metal-organic frameworks for enhanced carbon dioxide fixation
- Creator
- Sun, Xiaodong; Shi, Litong; Hu, Haijun; Huang, Hongwei; Ma, Tianyi
- Relation
- ARC
- Relation
- Advanced Sustainable Systems Vol. 4, Issue 9, no. 2000098
- Publisher Link
- http://dx.doi.org/10.1002/adsu.202000098
- Publisher
- Wiley-VCH Verlag GmbH
- Resource Type
- journal article
- Date
- 2020
- Description
- Ligand functionalization has always been considered as an effective method for regulating the catalytic activity of the metal-organic frameworks (MOFs) materials. Herein, three stable zirconium-based MOFs (Zr-MOFs), constructed by the 10-connected Zr6 cluster and different groups-decorated V-shaped ligands (H2L), are successfully synthesized through a facile ligand functionalization method. Subsequently, three isostructural Zr-MOFs, including the parent structure Zr(H2L), amino-decorated Zr(H2L) (NH2-Zr(H2L)), and fluorine and amino bi-decorated Zr(H2L) (F-NH2-Zr(H2L)), are employed as the platform for systematically investigating the effect of Lewis basic groups on the CO2 adsorption and separation behavior, more importantly the CO2 chemical fixation. Benefitting from the decorated Lewis basic groups, not only the CO2 adsorption enthalpy and selectivity over CH4 of NH2-Zr(H2L) and F-NH2-Zr(H2L) are improved, but also their catalytic activities for cycloaddition of CO2 to form cyclic carbonates are significantly enhanced. Among them, F-NH2-Zr(H2L) exhibits the most effective performance for cycloaddition of CO2 and styrene epoxide, which can be attributed to the strong polarization between the CO2 molecule and the framework of F-NH2-Zr(H2L). Under a mild condition, the yield of F-NH2-Zr(H2L) for cycloaddition of CO2 with styrene epoxide can reach up to 97%, which surpasses most of the reported MOFs-based catalysts.
- Subject
- CO2 fixation; ligand functionalization; Zr-MOFs; SDG 13; Sustainable Development Goals
- Identifier
- http://hdl.handle.net/1959.13/1435904
- Identifier
- uon:39855
- Identifier
- ISSN:2366-7486
- Language
- eng
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