Effect of Solvent Assisted Linker Exchange (SALE) and De Novo Synthetic Routes on CO 2 Uptake and Fixation by Mixed-Linker Zeolitic Imidazolate Frameworks
JOURNAL OF INORGANIC AND ORGANOMETALLIC POLYMERS AND MATERIALS(2023)
摘要
Direct mixing (de novo) and Solvent Assisted Ligand Exchange (SALE) are the main methods used for the synthesis of Mixed-Linker Zeolitic Imidazolate Frameworks (ML-ZIFs). ML-ZIFs with combined –NO 2 and –Br/–Cl functionalities were prepared via both synthetic routes. Thereafter the CO 2 uptake of the ML-ZIFs were compared, as well as their abilities to fixate CO 2 with epoxide substrates. The de novo synthesis resulted in ML-ZIFs with SOD topologies, 60: 40 (–NO 2 : –Br/–Cl) functionality ratios, higher porosities, better thermal stability and higher CO 2 uptake than equivalent SALE products. SALE resulted in smaller ML-ZIF crystallites, only ~ 10% incorporation of –Br/–Cl functionalized imidazolate linkers, and phase change during activation. ML-ZIF-7 Cl , obtained from direct mixing, resulted in the highest CO 2 uptake (90 cm 3 g −1 ), in line with its higher porosity. ML-ZIF-7 Cl , in combination with tetrabutylammonium bromide (TBAB), showed a high catalytic activity (TOF of 446 h −1 ) for the fixation of CO 2 with propylene oxide and was reusable for up to 4 cycles without loss in activity. Graphical Abstract
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关键词
Zeolitic imidazolate frameworks (ZIFs),Solvent assisted ligand exchange (SALE),De Novo synthesis,CO2 uptake,CO2 fixation
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