正丁胺和2-丁胺被H和OH自由基氧化的综合机理:对反应性的认识

IF 2.8 2区 化学 Q3 CHEMISTRY, PHYSICAL
Joel Leitão Nascimento, Tiago Vinicius Alves* and Yanlei Shang*, 
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引用次数: 0

摘要

本研究给出了一系列涉及1-和2-丁胺与关键自由基H和OH的抽氢反应的精确热速率常数。利用理论的M08-HX/ma-TZVP能级对这些反应产生的势能面进行了研究。采用带小曲率隧道修正的多结构典型变分理论(MS-CVT/SCT)计算速率系数。通过基于耦合扭转势(MS-T)的多结构方法计算的转振配分函数,评估了多结构效应和扭转非谐性修正。我们的结果证明了氨基官能团的位置对动力学的影响。随着氨基官能团与反应位点之间距离的增加,势垒高度逐渐降低。计算出的支链比表明,α-位点的H自由基更有利于H的抽离。在涉及OH自由基的反应中,n位的通道由于其增加的多结构扭转不谐性和减少的其他位置的变分效应而显示出更大的比例。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Comprehensive Oxidation Mechanism of n-Butylamine and 2-Butylamine by H and OH Radicals: Insights into Reactivity

This study presents the accurate thermal rate constants for a series of hydrogen abstraction reactions involving 1- and 2-butylamine and key radicals H and OH. The potential energy surface resulting from these reactions was examined by using the M08-HX/ma-TZVP level of theory. The rate coefficients were calculated within the multistructural canonical variational theory with small-curvature tunneling correction (MS-CVT/SCT). Multistructural effects and the torsional anharmonicity corrections were evaluated through the rovibrational partition function calculated with the multistructural method based on a coupled torsional potential (MS-T). Our results demonstrated an influence of the position of the amino functional group on the kinetics. The gradual decrease in barrier heights was observed with increasing distance between the amino functional group and the reaction site. The calculated branching ratios demonstrated that the H-abstraction by the H radicals at the α-site is favored. In reactions involving OH radicals, the channel at the N-site shows a greater proportion due to its increased multistructural torsional anharmonicity and a reduced variational effect of other sites.

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来源期刊
The Journal of Physical Chemistry A
The Journal of Physical Chemistry A 化学-物理:原子、分子和化学物理
CiteScore
5.20
自引率
10.30%
发文量
922
审稿时长
1.3 months
期刊介绍: The Journal of Physical Chemistry A is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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