Site- and conformer-specific reaction dynamics of glycine with the hydroxyl radical

甘氨酸与羟基自由基的位点和构象特异性反应动力学

阅读:3

Abstract

Understanding the state-to-state atomic-level dynamics of a chemical reaction is a central topic in modern chemistry. Moving beyond the traditional mode-specific reaction dynamics studies, here we investigate the concept of site and conformer specificity by studying the reaction of the glycine molecule (H(2)NCH(2)COOH) with the hydroxyl (OH) radical using first-principles theory. Conformer-specific quasi-classical trajectory computations on a 30-dimensional potential energy surface reveal three distinct H-abstraction pathways targeting the different functional groups. CH(2)- and NH(2)-H-abstraction proceed through direct, single-step mechanisms, whereas a two-step mechanism emerges for COOH-H-abstraction, where initial dehydrogenation frequently leads to fragmentation into CO(2) and CH(2)NH(2). COOH-H-abstraction is favored at low energies, while NH(2)- and CH(2)-H-abstraction are promoted at higher energies. The formation of the unstable H(2)NCH(2)COO• intermediate becomes increasingly restricted at higher collision energies due to limited interaction time. In specific reactant conformers, the simulations reveal an indirect biradical mechanism and an alternative stabilization pathway via intramolecular H transfer. Product-conformer distributions exhibit a three-step pattern of carboxyl group rearrangement-H-orientation switch, 180° rotation around the C-C axis, and their combination-during NH(2)- and CH(2)-H-abstraction. Structure-specific product formation arises clearly only in CH(2)-H-abstraction, driven by the closed COOH conformation, whereas NH(2)-H-abstraction leads to conformational diversity in the products.

特别声明

1、本页面内容包含部分的内容是基于公开信息的合理引用;引用内容仅为补充信息,不代表本站立场。

2、若认为本页面引用内容涉及侵权,请及时与本站联系,我们将第一时间处理。

3、其他媒体/个人如需使用本页面原创内容,需注明“来源:[生知库]”并获得授权;使用引用内容的,需自行联系原作者获得许可。

4、投稿及合作请联系:info@biocloudy.com。