D'Souza Malcolm J, Carter Shannon E, Kevill Dennis N
Department of Chemistry, Wesley College, 120 N. State Street, Dover, DE 19901, USA.
Int J Mol Sci. 2011 Feb 15;12(2):1161-74. doi: 10.3390/ijms12021161.
The specific rates of solvolysis of neopentyl chloroformate (1) have been determined in 21 pure and binary solvents at 45.0 °C. In most solvents the values are essentially identical to those for ethyl and n-propyl chloroformates. However, in aqueous-1,1,1,3,3,3-hexafluoro-2-propanol mixtures (HFIP) rich in fluoroalcohol, 1 solvolyses appreciably faster than the other two substrates. Linear free energy relationship (LFER) comparison of the specific rates of solvolysis of 1 with those for phenyl chloroformate and those for n-propyl chloroformate are helpful in the mechanistic considerations, as is also the treatment in terms of the Extended Grunwald-Winstein equation. It is proposed that the faster reaction for 1 in HFIP rich solvents is due to the influence of a 1,2-methyl shift, leading to a tertiary alkyl cation, outweighing the only weak nucleophilic solvation of the cation possible in these low nucleophilicity solvents.
在45.0°C下,已测定了新戊基氯甲酸酯(1)在21种纯溶剂和二元溶剂中的溶剂解比速率。在大多数溶剂中,其值与氯甲酸乙酯和正丙基氯甲酸酯的值基本相同。然而,在富含氟代醇的水 - 1,1,1,3,3,3 - 六氟 - 2 - 丙醇混合物(HFIP)中,1的溶剂解比其他两种底物快得多。将1的溶剂解比速率与氯甲酸苯酯和正丙基氯甲酸酯的溶剂解比速率进行线性自由能关系(LFER)比较,有助于机理研究,用扩展的格鲁纳德 - 温斯坦方程进行处理也是如此。有人提出,在富含HFIP的溶剂中1反应更快是由于1,2 - 甲基迁移的影响,导致形成叔烷基阳离子,在这些低亲核性溶剂中,这种影响超过了阳离子可能存在的唯一弱亲核溶剂化作用。