A detailed reaction mechanism for hexamethyldisiloxane combustion via experiments and ReaxFF molecular dynamics simulations

IF 1.5 4区化学 Q4 CHEMISTRY, PHYSICAL

International Journal of Chemical Kinetics Pub Date : 2023-10-17 DOI:10.1002/kin.21698

Yaosong Huang, Hao Chen

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引用次数: 0

Abstract

Hexamethyldisiloxane (HMDSO) is one of the main impurities in the syngas produced from sewage and landfill plants. In order to utilize this syngas or control the characteristics of the generated silica particles, it is crucial to understand the chemical kinetics of HMDSO combustion. This study investigated the process of HMDSO combustion using synchrotron radiation mass spectrometry (SRMS), gas chromatography (GC), and ReaxFF molecular dynamics simulations. First, the force field used for ReaxFF simulation was validated by comparing the energies of different bond lengths, bond angles, and dihedral angles with the ones from DFT calculations. Good agreements were found. Then, ReaxFF simulations of HMDSO combustion with this force field were conducted under various conditions, which include different equivalence ratios (0.67, 1.0, and 1.5) and temperatures ranging from 2000 to 3500 K. The oxidation characteristics of HMDSO were analyzed, including the evolution of gas products and particle formation. Finally, based on the results from experiments and ReaxFF simulations, the reaction pathways, reaction lists, and reaction kinetics data during HMDSO combustion were obtained. A detailed reaction mechanism was proposed and validated by applying it in modeling the H₂/HMDSO/O₂ combustion systems. The temperature and part of the gas products such as CO and CO₂ as well as SiO could be well predicted.

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通过实验和 ReaxFF 分子动力学模拟研究六甲基二硅氧烷燃烧的详细反应机理

六甲基二硅氧烷（HMDSO）是污水处理厂和垃圾填埋厂产生的合成气中的主要杂质之一。为了利用这种合成气或控制生成的二氧化硅颗粒的特性，了解 HMDSO 燃烧的化学动力学至关重要。本研究利用同步辐射质谱法（SRMS）、气相色谱法（GC）和 ReaxFF 分子动力学模拟研究了 HMDSO 的燃烧过程。首先，通过比较不同键长、键角和二面角的能量与 DFT 计算的能量，验证了 ReaxFF 模拟所用的力场。结果表明二者吻合良好。然后，利用该力场在不同条件下对 HMDSO 的燃烧进行了 ReaxFF 模拟，这些条件包括不同的当量比（0.67、1.0 和 1.5）和 2000 至 3500 K 的温度范围。最后，根据实验和 ReaxFF 模拟结果，获得了 HMDSO 燃烧过程中的反应路径、反应清单和反应动力学数据。通过对 H2/HMDSO/O2 燃烧系统建模，提出并验证了详细的反应机理。可以很好地预测 CO 和 CO2 等气体产物以及 SiO 的温度和部分含量。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

International Journal of Chemical Kinetics 化学-物理化学

CiteScore

3.30

自引率

6.70%

发文量

审稿时长

3 months

期刊介绍： As the leading archival journal devoted exclusively to chemical kinetics, the International Journal of Chemical Kinetics publishes original research in gas phase, condensed phase, and polymer reaction kinetics, as well as biochemical and surface kinetics. The Journal seeks to be the primary archive for careful experimental measurements of reaction kinetics, in both simple and complex systems. The Journal also presents new developments in applied theoretical kinetics and publishes large kinetic models, and the algorithms and estimates used in these models. These include methods for handling the large reaction networks important in biochemistry, catalysis, and free radical chemistry. In addition, the Journal explores such topics as the quantitative relationships between molecular structure and chemical reactivity, organic/inorganic chemistry and reaction mechanisms, and the reactive chemistry at interfaces.