期刊
FUEL
卷 332, 期 -, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2022.126191
关键词
Lewis pair; Poly(ionic liquid); CO2 conversion; Cyclic carbonate
This study proposes a one-step strategy to construct Lewis pair heterogeneous catalysts for CO2 conversion through the coordination of amino-functionalized poly(ionic liquid) and metal cations. The strength and ratio of Lewis acidic/basic sites can be tuned by regulating the type/content of metal ions, enabling efficient acid/base cooperation in CO2 cycloaddition. The synergistic effect of M2+, Br-, and C-2 proton on the imidazolium ring activates both CO2 and epoxides, leading to high yields and selectivity of cyclic carbonates under atmospheric pressure and low temperature without cocatalyst.
Lewis pair catalyst is considered to be a cutting-edge tool for the low-energy activation and subsequent conversion of CO2, which, yet suffers from complex preparation and unclear design strategy. This work proposes a one-step strategy for precisely constructing Lewis pair heterogeneous catalysts through the coordination of amino-functionalized poly(ionic liquid) (PIL) and metal cations for atmospheric CO2 conversion to cyclic carbonates. Self-tunability in the strength and ratio of Lewis acidic/basic sites is imparted by the facile regulation of the type/content of metal ions (Zn2+/Co2+/Cu2+), which is crucial for promoting acid/base cooperation in CO2 cycloaddition. The synergy of M2+, Br- and C-2 proton on imidazolium ring with an optimum acid/base molar ratio of ca. 1.47 has been proved to activate CO2 and epoxides synchronously, inducing a promising catalytic activity with high yield (similar to 95 %) and selectivity (>99 %) of cyclic carbonates under atmospheric pressure and low temperature (<= 75 degrees C) without cocatalyst.
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