星际分子1-氰基-1,3-丁二烯的气相合成机制研究

doi:10.3969/j.issn.1000-5641.2024.04.006

华东师范大学学报（自然科学版） ›› 2024, Vol. 2024 ›› Issue (4): 57-64.doi: 10.3969/j.issn.1000-5641.2024.04.006

星际分子1-氰基-1,3-丁二烯的气相合成机制研究

郑慧敏, 白西林, 龚起昂, 杨涛*()

华东师范大学精密光谱科学与技术国家重点实验室, 上海　200241

收稿日期:2023-04-13 接受日期:2023-05-19 出版日期:2024-07-25 发布日期:2024-07-23
通讯作者: 杨涛 E-mail:tyang@lps.ecnu.edu.cn
基金资助:
上海市自然科学基金 (22ZR1421400)

Gas phase formation mechanism of the interstellar molecule 1-cyano-1,3-butadiene

Huimin ZHENG, Xilin BAI, Qi’ang GONG, Tao YANG*()

State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai　200241, China

Received:2023-04-13 Accepted:2023-05-19 Online:2024-07-25 Published:2024-07-23
Contact: Tao YANG E-mail:tyang@lps.ecnu.edu.cn

摘要/Abstract

摘要：

为深入了解星际有机腈分子的动力学生成机制, 结合同步辐射真空紫外光电离实验和量子化学计算, 研究了高温星际环境中氰甲基自由基 (·CH₂CN) 与丙炔 (C₃H₄) 的反应机制. 通过分析光电离质谱与光电离效率图, 发现反应可能主要产生1-氰基-1,3-丁二烯开链异构体. 继而, 在B3LYP/cc-pVTZ水平上计算了反应势能面, 发现氰甲基自由基可无势垒地加成到丙炔上, 主要产生gauche-E-1-氰基-1,3-丁二烯和E-1-氰基-1,3-丁二烯这两种产物, 而热力学上更稳定的产物吡啶的生成概率较小.

关键词: 反应动力学, 1-氰基-1,3-丁二烯, 星际分子

Abstract:

In this study, a combination of synchrotron vacuum ultraviolet photoionization experiments and quantum chemical calculations was employed to investigate the reaction mechanism between cyanomethyl radicals (·CH₂CN) and propyne (C₃H₄) in high-temperature interstellar environments. The aim was to gain further insights into the formation mechanism of interstellar organic nitriles. By analyzing the photoionization mass spectra and photoionization efficiency curves, it was determined that the reaction may predominantly yield the open-chain isomers of 1-cyano-1,3-butadiene. Additionally, the reaction potential energy surface was explored at the B3LYP/cc-pVTZ level, revealing a barrierless addition of the cyanomethyl radical to acetylene. This addition mainly leads to the formation of gauche-E-1-cyano-1,3-butadiene and/or E-1-cyano-1,3-butadiene. Conversely, the more thermodynamically stable product, pyridine, exhibits a lower likelihood of formation.

Key words: reaction dynamics, 1-cyano-1,3-butadiene, interstellar molecules

中图分类号:

O561

郑慧敏, 白西林, 龚起昂, 杨涛. 星际分子1-氰基-1,3-丁二烯的气相合成机制研究[J]. 华东师范大学学报（自然科学版）, 2024, 2024(4): 57-64.

Huimin ZHENG, Xilin BAI, Qi’ang GONG, Tao YANG. Gas phase formation mechanism of the interstellar molecule 1-cyano-1,3-butadiene[J]. Journal of East China Normal University(Natural Science), 2024, 2024(4): 57-64.

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命名	相对能量 /(kJ/mol)	电离能/eV	命名	相对能量 /(kJ/mol)	电离能/eV
E-1-氰基-1,3-丁二烯	106.57	9.65	Z-1-氰基-1,3-丁二烯	107.65	9.65
4-氰基-1,2-丁二烯	176.98	10.00	4-氰基-1-丁炔	174.43	10.90
2-氰基-1,3-丁二烯	111.50	9.79	(氰基亚甲基) 环丙烷	188.57	10.22
1-氰基环丁烯	150.83	10.12	吡啶	0	9.35

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星际分子1-氰基-1,3-丁二烯的气相合成机制研究

Gas phase formation mechanism of the interstellar molecule 1-cyano-1,3-butadiene

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