TY - JOUR
T1 - Insight into the high-temperature oxidation kinetics of acetylene
T2 - A first-principles molecular dynamics study
AU - Zhang, Teng
AU - Shou, Liefeng
AU - Yang, Kun
AU - Long, Yao
AU - Chen, Lang
AU - Wang, Hongliang
AU - Chen, Jun
N1 - Publisher Copyright:
© 2024 Elsevier B.V.
PY - 2024/3/15
Y1 - 2024/3/15
N2 - The study on high-temperature oxidation kinetics and kinetic modeling of acetylene (C2H2) has significant importance for its engineering applications. In this paper, the first-principles molecular dynamics method is used to simulate the C2H2 oxidation under high temperatures for the first time. Our results show that there are 38 intermediates and 225 elementary reactions in the process of C2H2 oxidation. The formation mechanisms of “prompt” CO2, as well as gas pollutants CHOCHO and HCOOH are revealed in depth. Four intermediates, CHCHO, CHOCO, CHOCHO and HCOOH, which have significant controversy in current kinetic models, are verified. And a new intermediate, CHOCO2, is discovered. Meanwhile, our simulation also shows that radicals, such as HO2, OH, O, etc. play a key role in promoting the oxidation of intermediates in the early stage of C2H2 oxidation. Combined with quantum chemical calculations, a detailed chemical kinetic model of C2H2/air (FP-C2H2) is built and verified by simulating ignition delay time, species concentration in the flow reactor and premixed laminar flame speed. Our studies provide novel insight for understanding the complex chemical reaction kinetics, and environmental and human health threats from air pollutant formation during C2H2 combustion.
AB - The study on high-temperature oxidation kinetics and kinetic modeling of acetylene (C2H2) has significant importance for its engineering applications. In this paper, the first-principles molecular dynamics method is used to simulate the C2H2 oxidation under high temperatures for the first time. Our results show that there are 38 intermediates and 225 elementary reactions in the process of C2H2 oxidation. The formation mechanisms of “prompt” CO2, as well as gas pollutants CHOCHO and HCOOH are revealed in depth. Four intermediates, CHCHO, CHOCO, CHOCHO and HCOOH, which have significant controversy in current kinetic models, are verified. And a new intermediate, CHOCO2, is discovered. Meanwhile, our simulation also shows that radicals, such as HO2, OH, O, etc. play a key role in promoting the oxidation of intermediates in the early stage of C2H2 oxidation. Combined with quantum chemical calculations, a detailed chemical kinetic model of C2H2/air (FP-C2H2) is built and verified by simulating ignition delay time, species concentration in the flow reactor and premixed laminar flame speed. Our studies provide novel insight for understanding the complex chemical reaction kinetics, and environmental and human health threats from air pollutant formation during C2H2 combustion.
KW - C2H2 oxidation kinetics
KW - First-principles molecular dynamics
KW - Gas pollutant
UR - http://www.scopus.com/inward/record.url?scp=85184486627&partnerID=8YFLogxK
U2 - 10.1016/j.jhazmat.2024.133613
DO - 10.1016/j.jhazmat.2024.133613
M3 - Article
C2 - 38301439
AN - SCOPUS:85184486627
SN - 0304-3894
VL - 466
JO - Journal of Hazardous Materials
JF - Journal of Hazardous Materials
M1 - 133613
ER -