A strategy to overcome the thermodynamic limitation in CO2 conversion using ionic liquids and urea
A strategy to overcome the thermodynamic limitation in CO2 conversion using ionic liquids and urea
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DOI：
10.1039/c4gc02199a
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发表时间：
2015-03
期刊：
影响因子：
9.8
通讯作者：
Zhaofu Zhang;Congyi Wu;Jun Ma;Jinliang Song;H. Fan;Jinli Liu;Qinggong Zhu;B. Han
中科院分区：
文献类型：
--
作者：
Zhaofu Zhang;Congyi Wu;Jun Ma;Jinliang Song;H. Fan;Jinli Liu;Qinggong Zhu;B. Han
提高热力学上不利反应的平衡转化率是化学家们非常感兴趣和具有挑战性的课题。离子液体的独特性质为解决这一问题提供了新的机遇。本文提出了一种利用离子液体的可设计性和非挥发性来规避化学反应的热力学限制的策略。在这种方法中，反应物首先与功能性IL反应以形成高能IL中间体，其可以进一步与其他反应物反应以产生产物并再生IL。为了验证这种策略的可行性，碳酸二甲酯（DMC）和甲酸甲酯（MF）通过尿素的合成，这是非常重要的反应，用于转化CO2，但在化学上是不利的，进行了与二醇IL的援助。结果表明，该方法得到的DMC和MF的平衡产率分别比传统方法高64倍和9倍。
Enhancing the equilibrium conversion of thermodynamically unfavorable reactions is a very interesting and challenging topic for chemists. The unique properties of ionic liquids (ILs) provide new opportunities to solve this problem. Herein a strategy is proposed to circumvent the thermodynamic limitation of chemical reactions using the designable and non-volatile nature of ILs. In this approach a reactant first reacts with a functional IL to form a high energy IL intermediate, which can further react with other reactants to yield products and regenerate the IL. To verify the feasibility of this strategy, the syntheses of dimethyl carbonate (DMC) and methyl formate (MF) via urea, which are very important reactions used to convert CO2 but are thermodynamically unfavorable, were conducted with the aid of a diol IL. It was found that the equilibrium yields of DMC and MF obtained by this methodology could be 64 times and 9 times higher, respectively, than those of the conventional methods.