Construction of stable MOFs integrated with open metal sites and amine groups for CO2 capture and conversion

胺气处理 金属 化学 无机化学 金属有机骨架 材料科学 化学工程 有机化学 吸附 工程类
作者
Weixuan Chen,Weize Wang,Junjun Wang,Bo Liu,Huifang Zhou
出处
期刊:Journal of Solid State Chemistry [Elsevier]
卷期号:317: 123729-123729 被引量:1
标识
DOI:10.1016/j.jssc.2022.123729
摘要

CO 2 is deemed as the major greenhouse gas causing global warming over the past several decades. Developing porous solid materials to achieve the capture and utilization of CO 2 , in this work, two metal–organic frameworks (MOFs), [Ni 2 (5H-Ade)(TCPE)(H 2 O) 3 ]∙3DMF∙6H 2 O (Ni-Ade-TCPE), and [Co 4.5 (HCOO) 3 (4H-Ade) 2 (TCPE)(H 2 O) 5 ]·5DMF·7H 2 O (Co-Ade-TCPE) have been synthesized by employing mixed adenine and tetrakis(4-carboxyphenyl)ethylene (H 4 TCPE). The structural analysis demonstrates they are 3D frameworks possessing 1D open channels with –NH 2 groups and open metal sites modified surfaces. They display impressive chemical stability in acidic and basic water solutions and high adsorption capacity for CO 2 . At 70 °C and 1 bar, Ni-Ade-TCPE exhibits outstanding activity, selectivity, and recyclability in the cycloaddition reaction of epoxides with CO 2 due to Lewis acid–base bifunctional sites. Moreover, a reasonable catalytic reaction mechanism has been proposed. Two stable MOFs, Ni-Ade-TCPE and Co-Ade-TCPE, based on a mixed-ligand strategy were synthesized, which are 3D microporous structures with 1D open channels decorated by –NH 2 sites. They show good chemical stability in water, acidic and alkaline solutions, and high CO 2 uptake. Ni-Ade-TCPE exhibits high performances in catalyzing cycloaddition of CO 2 with epoxides under mild conditions. • Two MOFs with multiple functional sites have been synthesized based mixed ligands. • They display high chemical stabilities in acidic and basic aqueous solutions. • Ni-Ade-TCPE can efficiently catalyze the conversion of CO 2 with different epoxide.
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