Bio-based organic polyamides as a non-metal heterogeneous catalyst for the halide-free cycloaddition of carbon dioxide. (15th October 2022)

• Record Type: Journal Article
• Authors: Yue, Zhongxiao; Hu, Tianding; Su, Hongying; Zhao, Wenbo; Li, Yang; Zhao, Hui; Liu, Yunli; Liu, Yi; Zhang, Heng; Jiang, Lihong; Tang, Xiaoning; Shan, Shaoyun; Zhi, Yunfei
• Is Part Of: Fuel. Volume 326(2022)
• Publication Date: 2022-10-15
• Subjects: CO2 cycloaddition -- Bio-based -- Metal-free catalysis -- Heterogeneous catalyst -- Reaction kinetics -- Density functional theory; Fuel -- Periodicals; Coal -- Periodicals; Coal; Fuel; Periodicals; 662.6
• DOI: 10.1016/j.fuel.2022.125007
• Languages: English
• ISSNs: 0016-2361

Abstract

Graphical abstract: Novel sustainable bio-based catalyst featuring superior advantages in CO2 chemical conversion provides feasible schedule for alleviating the CO2 excessive emission in the air. Highlights: A novel bio-based heterogeneous catalyst (MFM-KUST) was synthesized by a facile "one-pot" polycondensation at ambient temperature. MFM-KUST exhibited higher catalytic performance in CO2 cycloaddition than the melamine derivatives catalysts or other bio-based catalysts. The CO2 cycloaddition was carried out in the absence of metal, halide/co-catalyst and solvent reaction conditions. MFM-KUST showed superior catalytic efficiency for the cycloaddition of CO2 with epichlorohydrin, glycidol and propylene oxide, respectively. The cycloaddition mechanism was proposed and verified based on experiment and DFT calculations. Abstract: An environmentally-friendly organic polyamide heterogeneous catalyst (MFM-KUST) was prepared from bio-based nitrogen-rich precursors through a facile "one-pot" polycondensation at ambient temperature. MFM-KUST, a novel non-metal catalyst, was applied to the cycloaddition of CO2 and epoxides into cyclic carbonates (maximum yield ∼98.8%) under halide- and solvent-free conditions. The chemical structures and properties of the catalysts prepared by different solvents were comprehensively evaluated by standard analytical techniques. The kinetics and cycle stability of MFM-KUST were investigated, in addition, the cycloaddition mechanism was proposed and verified based on experiment and density functional theory (DFT) calculations. The results showed that MFM-KUST had an excellent catalytic performance because of the synergistic effects between hydrogen bond donors (-N-H, C=O---H or =N---H), imino groups (-N=) of triazine-ring, and hydrazine group (N-H) with edge defects.