石油学报(石油加工) ›› 2019, Vol. 35 ›› Issue (6): 1130-1137.doi: 10.3969/j.issn.1001-8719.2019.06.012

• 研究报告 • 上一篇    下一篇

吡咯和吡啶燃烧的反应分子动力学模拟

冯炜,高红凤,刘婷,马琼,周慧,蔡文艺,白红存   

  1. 宁夏大学 省部共建煤炭高效利用与绿色化工国家重点实验室 化学化工学院,宁夏 银川 750021
  • 收稿日期:2018-10-08 修回日期:2018-12-06 出版日期:2019-11-25 发布日期:2020-01-16
  • 通讯作者: 白红存,男,副研究员,博士,从事复杂能源体系结构与反应性研究,Tel:0951-2062328,E-mail:hongcunbai@nxu.edu.cn E-mail:hongcunbai@gmail.com
  • 作者简介:冯炜,女,硕士研究生,从事能源化学工程相关研究,E-mail:1812939016@qq.com
  • 基金资助:
    宁夏自然科学基金面上项目(NZ17008)、宁夏重点研发重大科技项目(2018BCE01002)、宁夏高等学校一流学科建设项目(NXYLXK2017A04)资助

ReaxFF Molecular Dynamics Simulations of the Combustion Reactions ofPyrrole and Pyridine

FENG Wei, GAO Hongfeng, LIU Ting, MA Qiong, ZHOU Hui, CAI Wenyi, BAI Hongcun   

  1. State Key Laboratory of HighEfficiency Utilization of Coal and Green Chemical Engineering, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China
  • Received:2018-10-08 Revised:2018-12-06 Online:2019-11-25 Published:2020-01-16

摘要: 采用基于反应力场的分子动力学方法(ReaxFF)研究了吡咯和吡啶的燃烧反应机理。重点考察了不同温度下吡咯和吡啶的燃烧过程中反应物、产物和主要反应中间体的分子数量变化规律,基于动力学轨迹可视化地观察获得了吡咯和吡啶的燃烧反应机理。结果表明,温度是影响芳香氮化物燃烧的重要因素。在燃烧过程中,随着温度的升高,CO2、H2O和氮氧化物(NOx)的生成速率逐渐加快,数量增多。随着反应的进行,CO2和H2O的生成量会逐渐趋于平衡,且达到平衡的时间随温度的升高而加快。吡咯和吡啶的分解速率都随着温度的升高不断增大。但在相同温度下,吡啶的分解时间比吡咯要长,分解速率比吡咯要低。两者燃烧产物、氧化过程中的含氮中间体相同,但热解开环方式、烃类自由基裂解路径明显不同。

关键词: 分子模拟, 反应力场, 吡咯, 吡啶, 燃烧

Abstract: The mechanism of pyrrole and pyridine combustions was studied by means of the reactive force field molecular dynamic simulations. The number of reactants, products and main reaction intermediates during combustion processes were investigated at various temperatures. The mechanism was visually observed based on the kinetic trajectory analysis. The results show that the reactive temperature is an important factor that affects the combustion of aromatic nitrides. As temperature increases, the formation rates of CO2, H2O and NOx radually increase during the combustions. With the reaction proceeding, the amounts of CO2 and H2O gradually reach the equilibrium, and the time to reach the equilibrium decreases with the increase of temperatures. The decomposition rates of pyrrole and pyridine increase with the increase of temperature. However, the decomposition time of pyridine is longer than that of pyrrole at the same temperature, since the decomposition rate of pyridine is lower than that of pyrrole. The main products and nitrogencontaining intermediates during combustion processes are nearly the same for pyrrole and pyridine, but the ringopening mode and the hydrocarbon free radical cracking path are rather different.

Key words: molecular simulations, reactive force field, pyrrole, pyridine, combustion

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