Shang Yanlei, Luo S N
Energy Research Institute, Qilu University of Technology (Shandong Academy of Sciences), Jinan, Shandong, 250014, P. R. China.
School of Materials Science and Engineering, Southwest Jiaotong University, Chengdu, Sichuan, 610031, P. R. China.
Phys Chem Chem Phys. 2024 Jul 31;26(30):20167-20215. doi: 10.1039/d4cp02187h.
Amines, a class of prototypical volatile organic compounds, have garnered considerable interest within the context of atmospheric and combustion chemistry due to their substantial contributions to the formation of hazardous pollutants in the atmosphere. In the current energy landscape, the implementation of carbon-neutral energy and strategic initiatives leads to generation of new amine sources that cannot be overlooked in terms of the emission scale. To reduce the emission level of amines from their sources and mitigate their impact on the formation of harmful substances, a comprehensive understanding of the fundamental reaction kinetics during the degeneration process of amines is imperative. This perspective article first presents an overview of both traditional amine sources and emerging amine sources within the context of carbon peaking and carbon neutrality and then highlights the importance of H-abstraction reactions in understanding the atmospheric and combustion chemistry of amines from the perspective of reaction kinetics. Subsequently, the current experimental and theoretical techniques for investigating the H-abstraction reactions of amines are introduced, and a concise summary of research endeavors made in this field over the past few decades is provided. In order to provide accurate kinetic parameters of the H-abstraction reactions of amines, advanced kinetic calculations are performed using the multi-path canonical variational theory combined with the small-curvature tunneling and specific-reaction parameter methods. By comparing with the literature data, current kinetic calculations are comprehensively evaluated, and these validated data are valuable for the development of the reaction mechanism of amines.
胺类作为一类典型的挥发性有机化合物，由于其对大气中有害污染物形成的重大贡献，在大气化学和燃烧化学领域引起了广泛关注。在当前的能源格局下，碳中性能源的实施和战略举措导致产生了新的胺源，就排放规模而言不容忽视。为了降低胺类从源头上的排放水平并减轻其对有害物质形成的影响，全面了解胺类降解过程中的基本反应动力学势在必行。这篇综述文章首先概述了在碳达峰和碳中和背景下的传统胺源和新兴胺源，然后从反应动力学的角度强调了氢原子提取反应在理解胺类大气化学和燃烧化学中的重要性。随后，介绍了目前用于研究胺类氢原子提取反应的实验和理论技术，并简要总结了过去几十年来该领域的研究工作。为了提供胺类氢原子提取反应的准确动力学参数，使用多路径正则变分理论结合小曲率隧道效应和特定反应参数方法进行了先进的动力学计算。通过与文献数据比较，对当前的动力学计算进行了全面评估，这些经过验证的数据对于胺类反应机理的发展具有重要价值。
