《催化活化C-H键引发烷烃功能化的B3研究》-毕业论文（设计）.doc

催化活化C-H键引发烷烃功能化的B3研究 专业：应用化学 姓名： 学号： 指导老师： 摘要 本论文探讨的化学反应是，银配合物经过全氟化硼配体的催化反应：甲烷与重氮基醋酸酯生成丙酸乙酯。 利用超临界二氧化碳为溶剂是反应成功的关键。虽然催化剂只是保守的溶于CH4/CO2混合物,在40°C、 14小时以上收率达19%以上的丙酸乙酯。本文通过B3方法对反应物和产物进行理论计算，得出该反应相关的热力学数据（焓和吉布斯自由能等）、各原子所带电荷、HOMO、LOMO，从而计算出反应产率以及产物的空间构型。通过对热力学函数的计算我们得出反应的△r G＜0，从而判断该反应可自发进行。 关键字：重氮基醋酸酯；甲烷；B3；HOMO、LOMO；原子电荷 B3 study on Catalyze Functionalization of Alkanes via C-H Bond Activation Abstract This paper discussed the reaction is that silver complexes bearing perfluorinated indazolylborate ligands catalyze the reaction of methane (CH4) with ethyl diazoacetate (N2CHCO2Et) to yield ethyl propionate (CH3CH2CO2Et). The use of supercritical carbon dioxide (scCO2) as the solvent is key to the reaction ’s success. Although the catalyst is only sparingly soluble in CH4/CO2 mixtures, optimized conditions presently result in a 19% yield of ethyl propionate (based on starting quantity of the diazoester) at 40°C over 14 hours[1].We report here that we calculated reagent and product by B3 which we could get datum about thermodynamics(H,G) and atoms’ charge And then ,we worked out the productivity of reaction and molecular geometries of products. Through the calculation of thermodynamic functions we conclude that △r G＜0 and this reaction can be spontaneous. Keywords: ethyl diazoacetate；methane；B3；HOMO；LOMO；charge  目录 TOC \o 1-3 \h \z \u HYPERLINK \l _Toc322466561 第一章 绪论 PAGEREF _Toc322466561 \h 1 HYPERLINK \l _Toc322466562 1.1烷烃功能化的作用及其研究意义 PAGEREF _Toc322466562 \h 1 HYPERLINK \l _Toc322466563 1.2反应机理 PAGEREF _Toc322466563 \h 1 HYPERLINK \l _Toc322466564 第二章 B3计算 PAGEREF _Toc322466564 \h 2 HYPERLINK \l _Toc322466565 2.1研究体系 PAGEREF _Toc322466565 \h 2 HYPERLINK \l _Toc322466566 2.2计算数据及讨论 PAGEREF _Toc322466566 \h 3 HYPERLINK \l _Toc322466567 第三章电荷分析 PAGEREF _Toc322466567 \h 13 HYPERLINK \l _Toc322466568 第四章 结论 PAGEREF _Toc322466568 \h 17 HYPERLINK \l _Toc322466569 参考文献： PAGEREF _Toc322466569 \h 18 HYPERLINK \l _Toc3224665