TY - JOUR
T1 - Investigating the effects of helium, argon and hydrogen co-feeding on the non-oxidative coupling of methane in a dielectric barrier discharge reactor
AU - Maitre, Pierre Andre
AU - Long, James
AU - Bieniek, Matthew Simon
AU - Bannerman, Marcus N.
AU - Kechagiopoulos, Panagiotis
N1 - Acknowledgements
We acknowledge and greatly appreciate the assistance from Dr. Mihailova from Plasma Matters B.V. in working with the software Plasimo. The work was supported by the UK Engineering and Physical Sciences Research Council (EPSRC) New Investigator Award, grant no. EP/R031800/1. James Long was supported by a doctoral scholarship within the Leverhulme Centre for Doctoral Training in Sustainable Production of Chemicals and Materials (DS-2017-073).
PY - 2022/9/21
Y1 - 2022/9/21
N2 - The impact of helium, argon, and hydrogen co-feeding on methane non-oxidative coupling in dielectric barrier discharges is investigated in terms of reaction pathways and energy efficiency. One-dimensional fluid simulations are used to investigate short time-scales. Zero-dimensional global modelling, using inputs from the one-dimensional simulations, is utilised to study time-scales equivalent to those of experimental reactors. A previously developed detailed kinetic scheme for non-thermal methane plasma that accounts for the reactivity and relaxation of electronically and vibrationally excited species is extended to describe the interactions of noble gases with the species within the methane plasma. A wide range of compositions and applied voltages are studied to determine the conditions that improve the energy efficiency of methane conversion and the selectivity to value-added products. Penning dissociation has a significant impact in the case of mixtures with high content of argon, while hydrogen co-feeding increases selectivity towards ethane and ethylene versus acetylene.
AB - The impact of helium, argon, and hydrogen co-feeding on methane non-oxidative coupling in dielectric barrier discharges is investigated in terms of reaction pathways and energy efficiency. One-dimensional fluid simulations are used to investigate short time-scales. Zero-dimensional global modelling, using inputs from the one-dimensional simulations, is utilised to study time-scales equivalent to those of experimental reactors. A previously developed detailed kinetic scheme for non-thermal methane plasma that accounts for the reactivity and relaxation of electronically and vibrationally excited species is extended to describe the interactions of noble gases with the species within the methane plasma. A wide range of compositions and applied voltages are studied to determine the conditions that improve the energy efficiency of methane conversion and the selectivity to value-added products. Penning dissociation has a significant impact in the case of mixtures with high content of argon, while hydrogen co-feeding increases selectivity towards ethane and ethylene versus acetylene.
KW - Methane valorisation
KW - non-thermal plasma reactor
KW - kinetic modelling
KW - He
KW - Ar
KW - H2 co-feeding
U2 - 10.1016/j.ces.2022.117731
DO - 10.1016/j.ces.2022.117731
M3 - Article
VL - 259
JO - Chemical Engineering Science
JF - Chemical Engineering Science
SN - 0009-2509
M1 - 117731
ER -
