Fluid modelling of CO2 dissociation in a dielectric barrier discharge

Ponduri, Srinath; Becker, Markus M.; Welzel, S.; Sanden, van de Mcm Richard; Loffhagen, Detlef; Engeln, Richard

doi:10.1063/1.4941530

Cited by 83 publications

(82 citation statements)

References 70 publications

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“…The electrical energy dissipated in the gas discharge per period

E_{normalg} = P T

and the specific energy input

S E I = \frac{P}{V N_{normalm}} t_{normalr}

can directly be determined from the power dissipated in the DBD

P = \frac{1}{T} \int_{t_{0}}^{t_{0} + T} I (t) U_{normalg} (t) d t,

where N m = xN is the particle number density of the monomer HMDSO, and t r = V / F is the residence time of the gas mixture in the plasma zone with a volume of V = 0.8 cm 3 . The residence time amounts to t r = 8 ms, that is, about 690 periods, for the gas flow rate of F = 6 slm.…”

Section: Temporal Evolution Of Dbds In Ar–hmdso Mixturesmentioning

confidence: 99%

Impact of hexamethyldisiloxane admixtures on the discharge characteristics of a dielectric barrier discharge in argon for thin film deposition

Loffhagen

Becker

Czerny

et al. 2017

Contributions to Plasma Physics

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Atmospheric‐pressure dielectric barrier discharges (DBDs) in argon with admixtures of small amounts of hexamethyldisiloxane (HMDSO) have been analysed by means of numerical modelling. A time‐dependent, spatially one‐dimensional fluid‐Poisson model has been used, which takes into account the spatial variation of the discharge plasma between the plane‐parallel dielectrics covering the electrodes. Main features of the model, including the reaction kinetics for HMDSO, are given. Good agreement with related experimental studies of the ignition voltage for HMDSO amounts of up to 200 ppm and the temporal course of the discharge current for conditions typical of deposition experiments is obtained by the model calculations when assuming that 30% of the reactions of HMDSO with excited argon atoms, with a rate coefficient of 5.0 × 10−10 cm3/s, lead to the production of electrons due to Penning ionization. The modelling results for constant frequency f = 86.2 kHz and applied voltage Ua = 4 kV show that the electrical energy dissipated in the DBD decreases with an increasing amount of HMDSO and enable the determination of the energy absorbed per HMDSO molecule on the basis of their energy balance. The analysis of the plasma–chemical processes also makes clear that collision processes of HMDSO with excited argon atoms and molecules leading to neutral reaction products are essential for the formation of thin polymer films.

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“…The electrical energy dissipated in the gas discharge per period

E_{normalg} = P T

and the specific energy input

S E I = \frac{P}{V N_{normalm}} t_{normalr}

can directly be determined from the power dissipated in the DBD

P = \frac{1}{T} \int_{t_{0}}^{t_{0} + T} I (t) U_{normalg} (t) d t,

Section: Temporal Evolution Of Dbds In Ar–hmdso Mixturesmentioning

confidence: 99%

Impact of hexamethyldisiloxane admixtures on the discharge characteristics of a dielectric barrier discharge in argon for thin film deposition

Loffhagen

Becker

Czerny

et al. 2017

Contributions to Plasma Physics

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“…In recent years, several plasma chemistry models were presented in literature, for CO 2 splitting, CH 4 reforming, CO 2 /CH 4 , CH 4 /O 2 , CO 2 /H 2 O, CO 2 /H 2 , as well as CO 2 /N 2 or CH 4 /N 2 mixtures, because N 2 is one of the most important components in gas effluents. Note, however, that not all these studies were devoted to gas conversion applications.…”

Section: Introductionmentioning

confidence: 99%

Plasma based CO₂ and CH₄ conversion: A modeling perspective

Bogaerts

Bie

Snoeckx

et al. 2016

Plasma Processes & Polymers

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This paper gives an overview of our plasma chemistry modeling for CO 2 and CH 4 conversion in a dielectric barrier discharge (DBD) and microwave (MW) plasma. We focus on pure CO 2 splitting and pure CH 4 reforming, as well as mixtures of CO 2 /CH 4 , CH 4 /O 2 , and CO 2 /H 2 O. We show calculation results for the conversion, energy efficiency, and product formation, in comparison with experiments where possible. We also present the underlying chemical reaction pathways, to explain the observed trends. For pure CO 2 , a comparison is made between a DBD and MW plasma, illustrating that the higher energy efficiency of the latter is attributed to the more important role of the vibrational levels. K E Y W O R D S0D chemical kinetics model, CO 2 and CH 4 conversion, dielectric barrier discharges, microwave plasmas, plasma chemistry modeling | INTRODUCTIONIn recent years, there is increasing interest in plasma used for CO 2 and CH 4 conversion. Several types of plasma reactors are being investigated for this purpose, including (packed bed) dielectric barrier discharges (DBDs), [1][2][3][4][5][6][7][8][9][10][11][12][13][14] microwave (MW) plasmas, [15][16][17][18][19][20] ns-pulsed, [21] spark, [22][23][24] and gliding arc (GA) [25][26][27][28][29][30][31][32] discharges. Research focuses on pure CO 2 splitting into CO and O 2 , on CH 4 (and other hydrocarbons) reforming, and on mixtures of CO 2 with a hydrogen-source, that is, mainly CH 4 , but sometimes also H 2 O or H 2 , to produce value-added chemicals like syngas, hydrocarbons, and oxygenated products. Key performance indicators are the conversion and the energy efficiency of the process, as well as the possibility to produce specific value-added chemicals with good yields and selectivity. To realize the latter, the plasma should be combined with a catalyst (e.g., [3][4][5][6][7][8][9]33,34] ), as the plasma itself is a too reactive environment, and thus produces a wealth of reactive species, which easily recombine to form new molecules, without any selectivity.To improve the conversion, product yields and energy efficiency of this process, a good insight in the underlying plasma chemistry is crucial. This can be obtained by experiments, but measuring the reactive species densities inside the plasma is far from evident. Therefore, modeling of the plasma chemistry can be a valuable alternative, as it provides information on the most important chemical reaction pathways, and how to tune them to improve the conversion, energy efficiency, and product formation.In the 80s and 90s, some papers have been published on CO 2 plasma chemistry modeling, with applications to CO 2 lasers. [35][36][37] These models, however, did not consider the vibrational kinetics, which are important for energy efficient CO 2 conversion. [38] Some other papers have described the vibrational kinetics for gas flow applications, [39,40] but without focusing on the plasma chemistry. In 1981 Rusanov

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“…Combined with modelling studies of these streamers, the dynamics of discharges in DBDs is relatively well understood. This has allowed the modelling of complex chemistry in individual streamers [16], and subsequently in more complex fluid models [17]. This approach of studying spatially constrained discharges with catalysts is untested.…”

Section: Introductionmentioning

confidence: 99%

Plasma-catalyst interaction studied in a single pellet DBD reactor: dielectric constant effect on plasma dynamics

Butterworth

Allen

2017

Plasma Sources Sci. Technol.

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A novel single dielectric pellet DBD that is designed to facilitate studying the interaction between plasmas and catalysts is presented. The influence of material dielectric constant on plasma dynamics across a range of applied voltages is determined through the use of electrical characterisation combined with videos of the discharge. Different discharge modes in nitrogen are observed and their behaviour is characterised. A particular focus is given to the phenomenon known as 'partial discharging'. This is where incomplete plasma formation occurs between the electrodes of the reactor, which may have implications for the fair testing of catalysts in packed bed reactors. Additionally, the occurrence of an 'almond shaped' QV plot in the event of pointto-point discharging in PBRs is explained. This work provides easily implemented analytical techniques that can be applied to understand the behaviour of plasmas within packed bed DBD reactors.

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Fluid modelling of CO2 dissociation in a dielectric barrier discharge

Cited by 83 publications

References 70 publications

Impact of hexamethyldisiloxane admixtures on the discharge characteristics of a dielectric barrier discharge in argon for thin film deposition

Impact of hexamethyldisiloxane admixtures on the discharge characteristics of a dielectric barrier discharge in argon for thin film deposition

Plasma based CO₂ and CH₄ conversion: A modeling perspective

Plasma-catalyst interaction studied in a single pellet DBD reactor: dielectric constant effect on plasma dynamics

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Fluid modelling of CO2 dissociation in a dielectric barrier discharge

Cited by 83 publications

References 70 publications

Impact of hexamethyldisiloxane admixtures on the discharge characteristics of a dielectric barrier discharge in argon for thin film deposition

Impact of hexamethyldisiloxane admixtures on the discharge characteristics of a dielectric barrier discharge in argon for thin film deposition

Plasma based CO2 and CH4 conversion: A modeling perspective

Plasma-catalyst interaction studied in a single pellet DBD reactor: dielectric constant effect on plasma dynamics

Contact Info

Product

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Plasma based CO₂ and CH₄ conversion: A modeling perspective