Multiple-site activation induced by guanidine ionic liquid decorated chromium (III) terephthalate for coupling of carbon dioxide with epoxides

Nengjie Feng, Linyan Cheng, Yukun Zhang, Yujie Tao, Hui Wan, Chong Chen, Guofeng Guan

科研成果: 期刊稿件文章同行评审

摘要

Cycloaddition, as a sound strategy for high-value utilization of carbon dioxide (CO2), has been long pursued, wherein the challenging substrate activation process is a top priority for devising novel heterogeneous catalysts. In this study, a guanidine-based ionic liquid tethering –NH2 groups was designed and integrated with chromium (III) terephthalate (MIL-101(Cr)) through the coordination with unsaturated Cr3+ centers. The developed [NH2TMG]Br@MIL-101(Cr) (TMG represents tetramethylguanidine) decorated with plentiful basic functional groups created a fast channel for the capturing and binding of CO2, while the highly-accessible Lewis acidic sites (Cr3+) and hydrogen bond donors (N+-H) embedded within the nanocomposite synergized to activate the epoxide, synchronously. Under the reaction conditions optimized by response surface methodology (RSM) (103.2 °C, 1.03 MPa, 1.85 h, and 2.53 wt% of catalyst), a satisfactory chloropropene carbonate (CPC) yield of 98.2 % with a selectivity of 99.2 % were achieved. We further demonstrated the heterogeneity and recyclability of [NH2TMG]Br@MIL-101(Cr), and ascertained the substrate expansibility. Moreover, the in-situ diffuse reflectance infrared Fourier-transform spectra (DRIFTS) and density functional theory (DFT) computations afforded deep insights into the proposed multiple-site activation mechanism for CO2 coupling. This study highlighted an innovative pathway for constructing durable IL@MOFs nanocomposites and presented a tangible route to effectively converting CO2.

源语言英语
页(从-至)561-572
页数12
期刊Journal of Colloid and Interface Science
687
DOI
出版状态已出版 - 6月 2025

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