期刊
JOURNAL OF CO2 UTILIZATION
卷 36, 期 -, 页码 295-305出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.jcou.2019.10.021
关键词
CO2 cycloaddition; Cyclic carbonate; Epoxide; Quaternary phosphonium salt; Metal-organic framework
资金
- National Natural Science Foundation of China [51572119, 51662031]
- Distinguished Young Scientists program of Jiangxi Province [20162BCB23040]
Integration of synergic Lewis acid sites and nucleophilic anions that can facilitate ring-opening of epoxide is a good way to develop efficient catalyst for cycloaddition of CO2 with epoxides. Herein, we prepared a novel metal-organic framework (MOF) catalyst (Cr-MIL-101- [BuPh3P]Br) through grafting quaternary phosphonium salt ionic liquid (IL) on Cr-MIL-101 by a facile post-synthetic approach. The introduction of phosphonium salt IL highly improves the catalytic activity and stability compared with the parent Cr-MIL-101-NH2. In the absence of any solvent and co-catalyst, Cr-MIL-101- [BuPh3P]Br showed excellent catalytic activity for the cycloaddition reaction under moderate reaction conditions. Under optimized conditions, the yield and TOF of propylene carbonate can be achieved 97.8% and 1086.7 h(-1) , respectively. This is because the synergetic interaction of dual functional sites including Cr3+ as Lewis acid sites in MOF and Br(- )as nucleophile in IL could promote the ringopening of epoxide through the coordination of Cr3+ sites with O atom and the nucleophilic attack of Br on the less sterically hindered beta-carbon atom of epoxide, respectively. Comparison with other reported ILs-functionalized Cr-MIL-101 or other kinds of MOFs catalysts reveals that Cr-MIL-101- [BuPh3P]Br has superior catalytic performance and potential. Moreover, Cr-MIL-101-[BuPh3P]Br as a heterogeneous catalyst also showed good chemical stability and reusability.
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