甘油羧化生產碳酸甘油酯被認為是一種很有前途的方法，可以同時產生高價值的化學品與解決廢甘油和二氧化碳應用的問題。然而，目前甘油碳酸酯的選擇性和產率仍然很低。在我們的研究中，我們將環氧丙烷引入到甘油羧化反應中，以取代傳統的脫水劑。替代的甘油羧化反應涉及環加成和酯交換反應，在季銨基離子液體作為催化劑的存在下，該反應在熱力學上變得更加有利。含有不同陰離子（I-、Cl-）的季銨離子液體同時表現出路易斯酸性和鹼性的特性，其中含碘離子液體（PDBA-I）自聚合後的催化活性最好。在甲醇作為助催化劑的情況下加入 PDBA-I，可以在相對溫和的條件下（100°C和15 bar CO2）獲得高產率的碳酸甘油酯。 高活性可歸因於碘離子的強親核攻擊能力以加速環加成反應(速率決定步驟)。我們也提出了一種可能的反應機制來理解這項研究的反應路徑。這是首次使用季銨離子液體作為催化劑通過兩步反應增強甘油羧化高活性的路易斯酸性和鹼性性質的研究。

Glycerol carboxylation to produce glycerol carbonate has been considered a promising approach to simultaneously generate highly valuable chemicals and address the issue of waste glycerol and CO2 application. However, the selectivity and yield of glycerol carbon remained low at the current stage. In our study, we introduced propylene oxide to the glycerol carboxylation reaction to replace the conventional dehydration agent. The alternative glycerol carboxylation reaction involves a cycloaddition and transesterification reaction, which becomes more thermodynamically favorable in the presence of a quaternary ammonium ionic liquid as the catalyst. The quaternary ammonium ionic liquid containing different anions (I‒, Cl‒) exhibited both Lewis acidic and basic sites, and the iodine-containing ionic liquid (PDBA-I) had the best catalytic activity after self-polymerization. With the addition of PDBA-I in the presence of methanol as a co-catalyst, a high yield of glycerol carbon can be obtained at a relatively mild condition (100 °C and 15 bar of CO2). The high activity can be ascribed to the strong nucleophilic attack ability of the iodine ions to accelerate the cycloaddition reaction, which is the rate-determining step. A possible reaction mechanism was proposed to understand the reaction path in this work. This is the first study using a quaternary ammonium ionic liquid as a catalyst to strengthen Lewis acidic and basic properties for high activity of glycerol carboxylation through a two-step reaction.

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