乙酸基+O<sub>2</sub>及其分解异构化反应速率常数计算和不确定度分析

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乙酸基+O₂及其分解异构化反应速率常数计算和不确定度分析

更新时间：2025-07-09

- 乙酸基+O₂及其分解异构化反应速率常数计算和不确定度分析
- Issue 5, Pages: 109-117(2023)
- 作者机构：
  
  西安交通大学动力工程多相流国家重点实验室
- 作者简介：
- 基金信息：
- DOI：
  CLC： X701;TK401;O643.11
- Published：2023
- 稿件说明：
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[J]. 2023, (5): 109-117.
DOI：

[J]. 2023, (5): 109-117. DOI：

摘要

为了构建准确乙酸燃烧化学反应动力学模型，进行了乙酸基与O

及其分解异构化高精度的量子计算。利用CCSD（T）-F12/cc-pVTZ-F12//B2PLYPD3/cc-pVTZ算法，得到了反应体系势能面，并基于多参考态方法CASPT2/CBS//CASPT2/cc-pVTZ

获得无势垒反应势能面。通过气相单分子反应理论（RRKM）和主方程理论求解了温度和压力相关的速率常数，利用可变反应坐标过渡态理论求解无势垒反应乙酸基与O

加成反应的速率常数。结果表明：在低压或者高温条件下，超过99%的化学活化的O

H自由基直接分解为CH

H+CO

。随着压力升高，化学活化的O

H碰撞稳定后生成O

H则在后续反应中分解为CH

H+CO

。乙酸自由基在分解时，CO

+CH

产物通道占据主导地位。基于计算结果改进了原有乙酸模型，改进后的模型能够更好地预测层流燃烧速度，并且乙酸基存在更多的消耗路径，与量化计算结果一致。

Abstract

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references

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乙酸基+O2及其分解异构化反应速率常数计算和不确定度分析

DOI：

摘要

Abstract

关键词

Keywords

references

乙酸基+O₂及其分解异构化反应速率常数计算和不确定度分析