甲醇羰基化制乙酸催化剂结构的理论研究(Ⅱ)

Theoretical Study of the Catalyst Structure for Methanol Carbonylation to Acetic Acid(Ⅱ)

选定单体Ａ为４－乙烯基吡啶，采用以ＡＳＥＤ－ＭＯ（含原子对排斥的ＥＨＭＯ法）为基础的结构自动优化的ＥＨＴＯＰＴ法对甲醇羰基化制乙酸催化剂结构进行了理论研究。计算并比较了二元共聚物配体ＡＡ、ＡＢ（或ＢＡ）、ＢＢ分别与铑配位的成键状态、电荷布居及能量变化，进一步从理论上研究了甲醇羰基化制乙酸催化剂的结构，对实验得出的单体Ａ为４－乙烯基吡啶的共聚物为配体的催化剂活性不同于相应的２－乙烯基吡啶的结论给予了解释。

4vingl pyridine was chosen as ligand A to continue the theoritical study of the catalyst structure for methanol carbonylation to acetic acid used by the ASEDMO method(including atomic repellent energy).The conditions of bonds,charge distribution and energy change were compared for binary copolymer ligands AA,AB(or BA),BB combining with Rh.An explanation for the differenee of catalytical activities between 4vinglpynidine and 2vinglpynidine,which was shown experimentally,was given.