Acetic acid-assisted polyhydroxy acid modification of a zirconium-based MOF for synergistic CO2 fixation. Issue 6 (December 2022)

• Record Type: Journal Article
• Authors: Ma, Pan; Ding, Meili; Rong, Wei; Liu, Xi; Yao, Jianfeng
• Is Part Of: Journal of environmental chemical engineering. Volume 10:Issue 6(2022)
• Publication Date: 2022-12
• Subjects: UiO-66 -- Acid-promoted synthesis -- Defects -- Carbon dioxide -- Cyclic carbonate; Chemical engineering -- Environmental aspects -- Periodicals; Environmental engineering -- Periodicals; Chemical engineering -- Environmental aspects; Environmental engineering; Periodicals; 660.0286
• DOI: 10.1016/j.jece.2022.108739
• Languages: English
• ISSNs: 2213-2929

Abstract

Abstract: The synergistic catalysis involving multiple active sites provides a promising method for improved catalytic activity. In this work, we developed a gentle acetic acid-assisted polyhydroxy acid modification strategy to regulate the coordination environment of a zirconium-based MOF, UiO-66. D -gluconic acid with multiple hydroxyl groups is selected to replace the acetic acid coordinated at the metal nodes of UiO-66 via competitive coordination, allowing for the coexistence of hydrogen bonding donors and Lewis acid sites. The effect of acetic acid and D -gluconic acid separately as modulator and modifier agent to produce linker defects on catalytic properties of UiO-66 was investigated in the cycloaddition of carbon dioxide (CO2 ) with epichlorohydrin. It was demonstrated that the activity of UiO-66 can be tuned by the amount of D -gluconic acid. Remarkably, the resultant UiO-66-GA-1200, which is modified with 1200 μL of D -gluconic acid, achieves a high catalytic yield for CO2 cycloaddition of epichlorohydrin under 1 bar CO2 and 60 °C. In contrast of pure UiO-66, UiO-66-GA-1200 shows admirable catalytic activities (92–94% yield) even after exposure to humid environment or in simulated flue gas. This work provides a novel method for constructing MOF-based solid acid catalysts and casts a new light on the development of practical CO2 utilization. Graphical Abstract: ga1 Highlights: A series of zirconium-based MOFs containing multiple hydroxyl groups were prepared. UiO-66-GA-1200 has good catalytic activity for CO2 cycloaddition reaction. UiO-66-GA-1200 can be facilely separated by external magnetic field and reused. The catalytic activity can be well maintained under simulated flue gas conditions.