廉钰坤, 王春波, 洪迪昆. 掺氨对乙烯氧化过程中多环芳烃生成影响的分子动力学模拟[J]. 中国电机工程学报, 2025, 45(2): 461-468. DOI: 10.13334/j.0258-8013.pcsee.232127
引用本文: 廉钰坤, 王春波, 洪迪昆. 掺氨对乙烯氧化过程中多环芳烃生成影响的分子动力学模拟[J]. 中国电机工程学报, 2025, 45(2): 461-468. DOI: 10.13334/j.0258-8013.pcsee.232127
LIAN Yukun, WANG Chunbo, HONG Dikun. Molecular Dynamics Simulation of the Effect of Ammonia on the Generation of PAH During Ethylene Oxidation[J]. Proceedings of the CSEE, 2025, 45(2): 461-468. DOI: 10.13334/j.0258-8013.pcsee.232127
Citation: LIAN Yukun, WANG Chunbo, HONG Dikun. Molecular Dynamics Simulation of the Effect of Ammonia on the Generation of PAH During Ethylene Oxidation[J]. Proceedings of the CSEE, 2025, 45(2): 461-468. DOI: 10.13334/j.0258-8013.pcsee.232127

掺氨对乙烯氧化过程中多环芳烃生成影响的分子动力学模拟

Molecular Dynamics Simulation of the Effect of Ammonia on the Generation of PAH During Ethylene Oxidation

  • 摘要: 作为可再生能源的储能载体,氨与碳氢燃料掺混燃烧可实现大规模二氧化碳(CO2)减排。该文以多环芳烃(polycyclic aromatic hydrocarbons,PAH)重要前驱体乙烯为对象,采用反应分子动力学模拟方法研究掺氨对乙烯氧化过程中PAH生成的影响。结果表明,PAH的生成呈阶段特征,包括PAH的形成、生长和聚集成核过程。掺氨基本不影响PAH前驱体(C1-C5碳氢化合物)的生成和消耗,因此对PAH形成阶段的影响较小。掺氨导致含氮PAH分子的分解反应增强,进而抑制了PAH的生长,但掺氨基本不影响PAH的芳环结构分布。掺氨引入的N原子导致PAH分子间通过二维边界相互连接聚合的次数减少,但通过三维堆积产生的平行层结构增加,从而降低了PAH的稳定性。可知,掺氨抑制PAH生长的原因是PAH生长速度减慢以及PAH聚合的稳定性降低。

     

    Abstract: As a storage carrier for renewable energy, ammonia can be co-combusted with hydrocarbon fuel for large-scale reduction of CO2 emission. In this work, the effect of NH3 on polycyclic aromatic hydrocarbons (PAH) generation during ethylene oxidation is studied using the reactive molecular dynamics simulations. The results reveal that the generation of PAH exhibits a stage characteristic, which includes the formation, growth, and nucleation process of PAH. Ammonia addition does not significantly affect the generation and consumption of PAH precursors (C1-C5 hydrocarbons), and therefore has little impact on PAH formation. Ammonia addition enhances the decomposition reactions of nitrogen- containing PAH molecules, which in turn inhibits growth of PAH, but does not significantly affect the distribution of aromatic ring structures in PAH. The introduction of N atoms by ammonia addition leads to a decrease in the number of intermolecular connections between PAH molecules through two-dimensional boundaries. However, However, it promotes an increase in the parallel layer structure generated through three-dimensional stacking, thereby reducing the stability of PAH. In summary, the reason why ammonia doping inhibits the growth of PAH is that the growth rate of PAH slows down and the stability of PAH polymerization decreases.

     

/

返回文章
返回