尿素法合成2-咪唑啉酮中水催化作用的DFT研究

尿素法合成2-咪唑啉酮中水催化作用的DFT研究 Density Functional Theory Study on the Catalytic Effect of Water in the Synthesis of 2-Imidazolidinone by Urea Method 朱菲菲 ZHU Feifei 1 first-author 张运丰 ZHANG Yunfeng 1 张爱宏 ZHANG Aihong 1 陈磊 CHEN Lei 1 韩波 HAN Bo 1 周成冈 ZHOU Chenggang 1 吴金平 WU Jinping 1 中国地质大学可持续能源实验室,武汉 中国地质大学可持续能源实验室,武汉 Sustainable Energy Laboratory,China University of Geosciences Sustainable Energy Laboratory,China University of Geosciences 尿素法合成2-咪唑啉酮可以在常压下进行,而以水作溶剂可以显著提高2-咪唑啉酮的产率.本文采用第一原理密度泛函理论（DFT）计算方法对水在反应中的催化作用进行了研究.对有水以及无水条件下反应的路径及反应活化能的对比研究分析表明,无论是生成中间体还是生成产物的过程,水在反应系统中都不仅是作溶剂,它还能起到帮助质子转移,显著降低反应的活化能的作用. The yielding rate of 2-imidazolidinone can be significantly promoted when synthesized by urea method under ambient pressure using water as a solvent.In this paper,a study based on first-principle density functional theory（DFT） was reported on the catalytic effect of water in the synthetic process.By analyzing the reaction pathway and the activation energy of the reactions with/without water,we counld find that the water served not only as a solvent,but more importantly,as a proton transfer agent to remarkably decrease the activation energy towards either the intermediate or the final product. 尿素法 2-咪唑啉酮 水 密度泛函理论 urea method 2-imidazolidinone water density functional theory（DFT） 10.14188/j.1671-8836.2010.03.009 O621.2 国家自然科学基金资助项目（20873127） 2010-03-01 2021-04-01 3 56