Direct conversion of methanol to n-C4H10 and H2 in a dielectric barrier discharge reactor

Wang, Li; Liu, S. Y.; Xu, C.; Tu, Xin

doi:10.1039/c6gc01604a

Cited by 24 publications

(22 citation statements)

References 39 publications

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“…In non‐thermal plasmas, there is a significant difference in the temperature between the electrons and heavy particles. The overall gas kinetic temperature of a plasma can be as low as room temperature, while the produced electrons are highly energetic (e.g., 1–10 eV) and can break most chemical bonds within molecules (e.g., CH 4 ) as well as producing a variety of chemically reactive species: free radicals, excited atoms, ions and molecules for the initiation, and propagation of chemical reactions . The non‐equilibrium character of such plasmas could overcome thermodynamic barriers in chemical reactions and enable thermodynamically unfavorable reactions (e.g., biogas reforming) to occur under ambient conditions.…”

Section: Introductionmentioning

confidence: 99%

Plasma‐catalytic reforming of biogas over supported Ni catalysts in a dielectric barrier discharge reactor: Effect of catalyst supports

Mei

Ashford

et al. 2016

Plasma Processes & Polymers

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In this study, plasma-catalytic reforming of simulated biogas for the production of value-added fuels and chemicals (e.g., H 2 ) has been carried out in a coaxial dielectric barrier discharge (DBD) plasma reactor. The influence of four Ni catalysts (Ni/γ-Al 2 O 3 , Ni/MgO, Ni/SiO 2 , and Ni/TiO 2 ) on the plasma-catalytic biogas reforming has been investigated in terms of the conversion of reactants, the yield and selectivity of target products, the carbon deposition on the catalysts, and the energy efficiency of the plasma-catalytic process. The use of plasma combined with these Ni catalysts enhanced the performance of the biogas reforming. A maximum CO 2 conversion of 26.2% and CH 4 conversion of 44.1% were achieved when using the Ni/γ-Al 2 O 3 catalyst at a specific energy density (SED) of 72 kJ l −1 . Compared to other Ni catalysts, placing the Ni/γ-Al 2 O 3 catalyst in the DBD produced more syngas and C 3 ─C 4 hydrocarbons, but less C 2 H 6 . The lowest energy cost (EC) for biogas conversion and syngas production, as well as the highest energy efficiency and fuel production efficiency (FPE), were achieved when using the Ni/γ-Al 2 O 3 catalyst in the plasma process. The Ni/γ-Al 2 O 3 catalyst also showed the lowest surface carbon deposition of 3.8%, after catalysing the plasma biogas reforming process for 150 min at a SED of 60 kJ l −1 . Compared to other Ni catalysts, the enhanced performance of the Ni/γ-Al 2 O 3 catalyst can be attributed to its higher specific surface area, higher reducibility and more, stronger basic sites on the catalyst surface. K E Y W O R D Sbiogas reforming, dielectric barrier discharge, Ni catalysts, plasma-catalysis

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Section: Introductionmentioning

confidence: 99%

Plasma‐catalytic reforming of biogas over supported Ni catalysts in a dielectric barrier discharge reactor: Effect of catalyst supports

Mei

Ashford

et al. 2016

Plasma Processes & Polymers

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“…According to Figure , over the temperature range investigated in this study, reactions 8 and 9 are the two energetically favorable methanol dissociation pathways and they occur spontaneously at T > 3200 K. Although reaction 7 is not energetically feasible in the investigated temperature range and reactions 8 and 9 are favored only in a narrow temperature range, processes such as ultrasound, electrical discharge plasma, and thermal cracking are usually sufficient sources of energy necessary for reactions 7–9 to proceed.…”

Section: Discussionmentioning

confidence: 62%

“…In the presence of water, CO is converted to CO 2 via the gas‐water shift reaction (reaction 5), which is the main reaction pathway for the production of CO 2 . Thus, if methanol and water are both present, reaction 6 will be the primary pathway for methanol decomposition

C {normalH}_{3} O H \to C O + 2 {normalH}_{2}

C O + {normalH}_{2} O \to C {normalO}_{2} + {normalH}_{2}

C {normalH}_{3} O H + {normalH}_{2} O \to C {normalO}_{2} + 3 {normalH}_{2}

…”

Section: Discussionmentioning

confidence: 79%

“…Ethanol, which has been detected previously in the literature can be formed from different precursors (reactions S3.1‐S3.6 in Table S3 and Figures S22 and S23). At temperatures <2000 K, ethanol can be formed from methyl and hydroxymethyl radicals (reaction 36).…”

Section: Discussionmentioning

confidence: 88%

“…The gas products that were detected include H 2 , CO, CH 4 , CO 2 , C 2 H 2 , C 2 H 4 , and C 2 H 6 . The primary chemical reactions in methanol plasmas responsible for these products are assumed to take place via electron excitation and electron impact dissociation both of which require energies below 10 eV and result in the dissociation of CH, OH, and CO bonds. Concurrently, very high temperatures (1000 K and higher) that are characteristic of streamer‐like plasmas enable thermal decomposition of molecules .…”

Section: Discussionmentioning

confidence: 99%

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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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methanol‐to‐gasoline process

Subramaniam¹

2020

Catalysis From a to Z

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Direct conversion of methanol to n-C₄H₁₀ and H₂ in a dielectric barrier discharge reactor

Abstract: A direct conversion of methanol to n-C4H10 and H2 by limiting CO and CO2 formation was achieved in a coaxial dielectric barrier discharge plasma reactor without a catalyst.

Cited by 24 publications

References 39 publications

Plasma‐catalytic reforming of biogas over supported Ni catalysts in a dielectric barrier discharge reactor: Effect of catalyst supports

Plasma‐catalytic reforming of biogas over supported Ni catalysts in a dielectric barrier discharge reactor: Effect of catalyst supports

Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol

methanol‐to‐gasoline process

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Direct conversion of methanol to n-C4H10 and H2 in a dielectric barrier discharge reactor

Abstract: A direct conversion of methanol to n-C4H10 and H2 by limiting CO and CO2 formation was achieved in a coaxial dielectric barrier discharge plasma reactor without a catalyst.

Cited by 24 publications

References 39 publications

Plasma‐catalytic reforming of biogas over supported Ni catalysts in a dielectric barrier discharge reactor: Effect of catalyst supports

Plasma‐catalytic reforming of biogas over supported Ni catalysts in a dielectric barrier discharge reactor: Effect of catalyst supports

­­Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol

methanol‐to‐gasoline process

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Product

Resources

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Direct conversion of methanol to n-C₄H₁₀ and H₂ in a dielectric barrier discharge reactor

Chemical reaction mechanisms accompanying pulsed electrical discharges in liquid methanol