链接剂缺陷辅助催化固定双链接剂金属有机框架中的二氧化碳

IF 1.7 4区 化学 Q4 CHEMISTRY, PHYSICAL Reaction Kinetics, Mechanisms and Catalysis Pub Date : 2024-05-31 DOI:10.1007/s11144-024-02656-4
Yunjang Gu, Sunghyun Yoon, Robin Babu, Yongchul G. Chung, Dae-Won Park
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引用次数: 0

摘要

我们研究了通过回收具有双链接器的金属有机框架 MOF-508 引发的链接器缺陷对催化 CO2 环加成反应的影响。采用粉末 XRD、FT-IR、FE-SEM、HR-TEM、TGA、BET、NH3- 和 CO2-TPD、NMR 和 CO2 吸附等温线等多种分析技术对 MOF-508 催化剂进行了表征。在无溶剂和中等反应条件下,MOF-508 催化剂可以进行环氧化物与 CO2 的偶联反应,对环碳酸盐的选择性高达 99%。环加成反应后,在所有温度范围内,回收的 MOF-508 都比新制备的 MOF-508 表现出更高的催化活性。循环催化活性提高的原因是连接体缺陷产生了额外的催化活性位点。研究人员利用分子建模技术阐明了催化机理,并对 MOF-508 中的链接缺陷程度进行了量化。
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Linker-defect assisted catalytic fixation of CO2 in a dual-linker metal–organic framework

We investigated the effect of linker defects induced by recycling MOF-508, a metal–organic framework with dual linkers, for the catalytic cycloaddition of the CO2 reaction. MOF-508 catalysts are characterized using various analytical techniques such as powder XRD, FT-IR, FE-SEM, HR-TEM, TGA, BET, NH3- and CO2-TPD, NMR, and CO2 adsorption isotherm. MOF-508 catalysts could perform the coupling reaction between epoxide and CO2 with > 99% selectivity toward cyclic carbonates under solvent-free and moderate reaction conditions. After the cycloaddition reaction, the recycled MOF-508 exhibited higher catalytic activity than freshly prepared MOF-508 at all the temperature ranges. The origin of increased cyclic catalytic activities was attributed to the creating of additional catalytic active sites from the linker defects. Molecular modeling techniques were used to elucidate the catalytic mechanism and quantify the degree of linker defects in MOF-508.

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来源期刊
CiteScore
3.30
自引率
5.60%
发文量
201
审稿时长
2.8 months
期刊介绍: Reaction Kinetics, Mechanisms and Catalysis is a medium for original contributions in the following fields: -kinetics of homogeneous reactions in gas, liquid and solid phase; -Homogeneous catalysis; -Heterogeneous catalysis; -Adsorption in heterogeneous catalysis; -Transport processes related to reaction kinetics and catalysis; -Preparation and study of catalysts; -Reactors and apparatus. Reaction Kinetics, Mechanisms and Catalysis was formerly published under the title Reaction Kinetics and Catalysis Letters.
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