Analysis of a Methanol Decomposition Process by a Nonthermal Plasma Flow

Sato, Takehiko; Kambe, Makoto; Nishiyama, Hideya

doi:10.1299/jsmeb.48.432

Cited by 15 publications

(15 citation statements)

References 20 publications

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“…Acetic acid, allyl alcohol, 1‐propanol, 3‐buten‐1‐ol, 3‐butyn‐1‐ol, glycolaldehyde, and methyl glycolate are produced through complex reactions with methanol and its degradation products. This may indicate why these products were not detected in previous studies of methanol in plasma …”

Section: Discussionsupporting

confidence: 87%

“…Figure summarizes the plasma‐assisted degradation of liquid methanol, based on the products identified and most feasible reactions. The proposed reaction mechanism is similar to previously proposed reaction schemes for plasmas in gaseous methanol and methanol pyrolysis, but with noticeable differences in product types . Due to the existence of large plasma temperature gradients and the fact that the plasma is surrounded by liquid methanol, our study additionally detected larger gas hydrocarbons and C 1 –C 4 liquid products.…”

Section: Discussionmentioning

confidence: 97%

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Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol

Franclemont

Fan

et al. 2018

Plasma Processes & Polymers

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The primary goal of this study was to explore the fundamental chemical processes occurring during a pulsed electrical discharge in liquid methanol. To this end, advanced analytical techniques were used to identify and, when possible, quantify gas and liquid methanol decomposition products. The effects of applied voltage, voltage polarity, and presence of water on the reaction stoichiometry and the selectivity for the identified gas products were also studied. Density Functional Theory (DFT) simulations were used to determine the most feasible thermal reaction pathways between 300 and 4000 K responsible for the formation of experimentally identified gas and liquid products. From these results, the key chemical reaction pathways were theorized and a reaction mechanism was developed. Gas products of plasmainduced decomposition of methanol that were detected and quantified include hydrogen, carbon monoxide, carbon dioxide, methane, acetylene, ethylene, and ethane. The reaction selectivity was the highest for the former two compounds regardless of the applied voltage, discharge polarity or presence of water in the starting solution. Results also showed that the applied voltage, discharge polarity and presence of water had no effect on the types of reaction products.Liquid methanol decomposition products that where identified include ethanol, ethylene glycol, formaldehyde, acetic acid, allyl alcohol, 1-propanol, 3-buten-1-ol, 3-butyn-1-ol, glycolaldehyde, and methyl glycolate. The chemical reaction mechanism that was proposed to explain the formation of the experimentally verified gas products offers specific pathways for the production of carbon monoxide and short-chained hydrocarbons. In contrast, the reactions leading to the formation of hydrogen, carbon dioxide, and liquid products appear to be random.

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Section: Discussionsupporting

confidence: 87%

Section: Discussionmentioning

confidence: 97%

Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol

Franclemont

Fan

et al. 2018

Plasma Processes & Polymers

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“…In the present study, HCOH prefers to bind at the bridge sites of Ga 3 Ni 5 (111) surface, with the plane of the structure formed vertical to the step edge. Hydroxymethyl (H 2 COH) can be generated from HCOH or H 2 CO hydrogenation, which was proposed by a few scholars. ,,, CH 2 OH was also experimentally considered as an intermediate in CH 3 OH decomposition . Methoxy (CH 3 O) has also been experimentally detected as an intermediate on Cu catalysts , and is considered as an intermediate in CH 3 OH decomposition on Cu 2 O(111) surface .…”

Section: Resultsmentioning

confidence: 97%

Thermodynamic and Kinetic Study on Carbon Dioxide Hydrogenation to Methanol over a Ga₃Ni₅(111) Surface: The Effects of Step Edge

et al. 2018

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Density functional theory (DFT) was used to study the mechanisms of carbon dioxide (CO2) hydrogenation to methanol (CH3OH) on a stepped Ga3Ni5(111) surface. Surface properties, adsorption energies of reactants, and potential intermediates and products, as well as thermodynamic and kinetic parameters of elementary steps, were calculated. It is found that a stepped Ga3Ni5(111) surface with low surface energy not only can highly activate CO2 but also is beneficial to dissociative H2 adsorption. Moreover, the reactants, intermediates, and products on the Ga3Ni5(111) surface prefer to adsorb to Ni sites at step edges. Accoring to calculated thermodynamic and kinetic parameters of all the elementary steps, CO2 is hydrogenated to CH3OH via trans-COOH, COHOH, COH, HCOH, and CH2OH intermediates because this pathway has the lowest activation barriers and highest rate constants. Meanwhile, water (H2O) formation is the rate-limiting step. On the basis of microkinetic modeling, Ga3Ni5(111) shows higher selectivity to CH3OH than CH4. In all, the stepped Ga3Ni5(111) surface is beneficial in facilitating CO2 hydrogenation to CH3OH, and the presence of steps and the existence of Ga on those steps instead of step edge are required for the high activity of the Ga3Ni5 catalyst.

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“… 5 Therefore, the generation of higher discharges in dry air plasma can lead to the formation of excited species such as O-radicals, excited N 2 and metastable . 13 This resulted in a more significant increase in the conversion of methanol.…”

Section: Resultsmentioning

confidence: 99%

Plasma-assisted removal of methanol in N₂, dry and humidified air using a dielectric barrier discharge (DBD) reactor

et al. 2022

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Analysis of a Methanol Decomposition Process by a Nonthermal Plasma Flow

Cited by 15 publications

References 20 publications

Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol

Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol

Thermodynamic and Kinetic Study on Carbon Dioxide Hydrogenation to Methanol over a Ga₃Ni₅(111) Surface: The Effects of Step Edge

Plasma-assisted removal of methanol in N₂, dry and humidified air using a dielectric barrier discharge (DBD) reactor

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Analysis of a Methanol Decomposition Process by a Nonthermal Plasma Flow

Cited by 15 publications

References 20 publications

­­Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol

­­Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol

Thermodynamic and Kinetic Study on Carbon Dioxide Hydrogenation to Methanol over a Ga3Ni5(111) Surface: The Effects of Step Edge

Plasma-assisted removal of methanol in N2, dry and humidified air using a dielectric barrier discharge (DBD) reactor

Contact Info

Product

Resources

About

Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol

Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol

Thermodynamic and Kinetic Study on Carbon Dioxide Hydrogenation to Methanol over a Ga₃Ni₅(111) Surface: The Effects of Step Edge

Plasma-assisted removal of methanol in N₂, dry and humidified air using a dielectric barrier discharge (DBD) reactor