Non-metal and non-halide enol PENDI catalysts for the cycloaddition of CO2 and epoxide. (September 2022)

• Record Type: Journal Article
• Authors: Liu, Yunli; Hu, Shuai; Zhi, Yunfei; Hu, Tianding; Yue, Zhongxiao; Tang, Xiaoning; Shan, Shaoyun
• Is Part Of: Journal of CO₂ utilization. Volume 63(2022)
• Publication Date: 2022-09
• Subjects: β-Diketone -- PENDIs -- Cycloaddition -- Non-metal Catalyst -- Carbon Dioxide; Carbon dioxide -- Periodicals; Carbon dioxide -- Environmental aspects -- Periodicals; Carbon dioxide mitigation -- Periodicals; Carbon dioxide; Carbon dioxide -- Environmental aspects; Carbon dioxide mitigation; Periodicals; 628.53205
• DOI: 10.1016/j.jcou.2022.102130
• Languages: English
• ISSNs: 2212-9820

Abstract

Abstract: A series of non-metal and high-efficiency PENDIs with hydrogen bond donor, which were prepared by condensation reaction of β-diketone and imine, are used for cycloaddition of CO2 and epoxides. The influences of different structure of catalysts and hydrogen bonds on catalytic performance were studied by experiments and density functional theory. The results showed that PENDIs which possess -OH of β-diketone and -NH- exhibit excellent catalytic performance for cycloaddition of CO2 and epichlorohydrin, and the record yield is 97.26 %. The single factor investigation and response surface methodology were used for obtaining optimal reaction conditions of PENDIs. A possible mechanism for CO2 cycloaddition that catalyzed by PENDIs is proposed, it includes epoxide adsorption, ring-opening of epoxide, CO2 insertion and the formation of cyclic carbonate. It is proved that the synergy between -OH of β-diketone and -NH- can promote the catalytic performance of PENDIs for CO2 cycloaddition. Graphical Abstract: Cycloaddition of CO2 with epoxide to synthesis the cyclic carbonate product is crucial due to the severe harm to the environment of CO2 and the wide application of the cyclic carbonate product. ga1 Highlights: A series of novel, non-metal PENDIs are successfully designed for the first time. The hydrogen bonds of -OH and -NH- of PENDIs were studied in detail. The synergy of hydrogen bonds of PENDI exhibits an excellent catalytic performance. DFT proved that the adsorptive influence of -OH on epoxide is stronger than -NH-. The possible mechanism of CO2 cycloaddition over PENDI catalysts was investigated.