Ab initio calculations and kinetic modeling of thermal conversion of methyl chloride: implications for gasification of biomass

Research output: Contribution to journalJournal article – Annual report year: 2018Researchpeer-review

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Ab initio calculations and kinetic modeling of thermal conversion of methyl chloride: implications for gasification of biomass. / Singla, Mallika; Rasmussen, Morten Lund; Hashemi, Hamid; Wu, Hao; Glarborg, Peter; Pelucchi, Matteo; Faravelli, Tiziano; Marshall, Paul.

In: Physical Chemistry Chemical Physics, Vol. 20, No. 16, 2018, p. 10741-10752.

Research output: Contribution to journalJournal article – Annual report year: 2018Researchpeer-review

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Singla, Mallika ; Rasmussen, Morten Lund ; Hashemi, Hamid ; Wu, Hao ; Glarborg, Peter ; Pelucchi, Matteo ; Faravelli, Tiziano ; Marshall, Paul. / Ab initio calculations and kinetic modeling of thermal conversion of methyl chloride: implications for gasification of biomass. In: Physical Chemistry Chemical Physics. 2018 ; Vol. 20, No. 16. pp. 10741-10752.

Bibtex

@article{6f9c92a450e048a684b4d41600c8fa8f,
title = "Ab initio calculations and kinetic modeling of thermal conversion of methyl chloride: implications for gasification of biomass",
abstract = "Limitations in current hot gas cleaning methods for chlorine species from biomass gasification may be a challenge for end use such as gas turbines, engines, and fuel cells, all requiring very low levels of chlorine. During devolatilization of biomass, chlorine is released partly as methyl chloride. In the present work, the thermal conversion of CH3Cl under gasification conditions was investigated. A detailed chemical kinetic model for pyrolysis and oxidation of methyl chloride was developed and validated against selected experimental data from the literature. Key reactions of CH2Cl with O2 and C2H4 for which data are scarce were studied by ab initio methods. The model was used to analyze the fate of methyl chloride in gasification processes. The results indicate that CH3Cl emissions will be negligible for most gasification technologies, but could be a concern for fluidized bed gasifiers, in particular in low-temperature gasification. The present work illustrates how ab initio theory and chemical kinetic modeling can help to resolve emission issues for thermal processes in industrial scale.",
author = "Mallika Singla and Rasmussen, {Morten Lund} and Hamid Hashemi and Hao Wu and Peter Glarborg and Matteo Pelucchi and Tiziano Faravelli and Paul Marshall",
year = "2018",
doi = "10.1039/C7CP07552A",
language = "English",
volume = "20",
pages = "10741--10752",
journal = "Physical Chemistry Chemical Physics",
issn = "1463-9076",
publisher = "Society of Chemical Industry - The Royal Society of Chemistry",
number = "16",

}

RIS

TY - JOUR

T1 - Ab initio calculations and kinetic modeling of thermal conversion of methyl chloride: implications for gasification of biomass

AU - Singla, Mallika

AU - Rasmussen, Morten Lund

AU - Hashemi, Hamid

AU - Wu, Hao

AU - Glarborg, Peter

AU - Pelucchi, Matteo

AU - Faravelli, Tiziano

AU - Marshall, Paul

PY - 2018

Y1 - 2018

N2 - Limitations in current hot gas cleaning methods for chlorine species from biomass gasification may be a challenge for end use such as gas turbines, engines, and fuel cells, all requiring very low levels of chlorine. During devolatilization of biomass, chlorine is released partly as methyl chloride. In the present work, the thermal conversion of CH3Cl under gasification conditions was investigated. A detailed chemical kinetic model for pyrolysis and oxidation of methyl chloride was developed and validated against selected experimental data from the literature. Key reactions of CH2Cl with O2 and C2H4 for which data are scarce were studied by ab initio methods. The model was used to analyze the fate of methyl chloride in gasification processes. The results indicate that CH3Cl emissions will be negligible for most gasification technologies, but could be a concern for fluidized bed gasifiers, in particular in low-temperature gasification. The present work illustrates how ab initio theory and chemical kinetic modeling can help to resolve emission issues for thermal processes in industrial scale.

AB - Limitations in current hot gas cleaning methods for chlorine species from biomass gasification may be a challenge for end use such as gas turbines, engines, and fuel cells, all requiring very low levels of chlorine. During devolatilization of biomass, chlorine is released partly as methyl chloride. In the present work, the thermal conversion of CH3Cl under gasification conditions was investigated. A detailed chemical kinetic model for pyrolysis and oxidation of methyl chloride was developed and validated against selected experimental data from the literature. Key reactions of CH2Cl with O2 and C2H4 for which data are scarce were studied by ab initio methods. The model was used to analyze the fate of methyl chloride in gasification processes. The results indicate that CH3Cl emissions will be negligible for most gasification technologies, but could be a concern for fluidized bed gasifiers, in particular in low-temperature gasification. The present work illustrates how ab initio theory and chemical kinetic modeling can help to resolve emission issues for thermal processes in industrial scale.

U2 - 10.1039/C7CP07552A

DO - 10.1039/C7CP07552A

M3 - Journal article

VL - 20

SP - 10741

EP - 10752

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

SN - 1463-9076

IS - 16

ER -