Investigating the Plasma-Assisted and Thermal Catalytic Dry Methane Reforming for Syngas Production: Process Design, Simulation and Evaluation

Delikonstantis, Evangelos; Scapinello, Marco; Stefanidis, Georgios D.

doi:10.3390/en10091429

Cited by 28 publications

(14 citation statements)

References 73 publications

(87 reference statements)

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“…Aspen Plus software (Version 8.4, Aspen Technology, Inc., Bedford, MA, USA) contains lots of different physical methods selectively applied to various conditions and materials with diverse characteristics [20][21][22][23][24][25]. In this report, the raw materials are mainly isobutylene, methanol, and air, where the gas phase conforms to Henry's Law of the ideal gas and the gas law, and the liquid phase belongs to a non-ideal system.…”

Section: Thermodynamic Methods Determinationmentioning

confidence: 99%

Design and Optimization of a Process for the Production of Methyl Methacrylate via Direct Methylation

et al. 2019

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Methyl methacrylate (MMA) plays a vital role in national productions with broad application. Herein, the production of MMA is realized by the improved eco-friendly direct methylation method using Aspen Plus software. Three novel kinds of energy-saving measures were proposed in this study, including the recycle streams of an aqueous solution, methacrolein (MAL), and methanol, the deployment of double-effect distillation instead of a normal one, and the design of a promising heat-exchange network. Moreover, MMA with a purity of 99.9% is obtained via the design of a MAL absorber column with an optimal stage number of 11 and a facile chloroform recovery process by using the RadFrac model. Thus, the proposed green process with energy-conservation superiority is the vital clue for developing MMA, and provides a reference for the production of MMA-ramifications with excellent prospects.Processes 2019, 7, 377 2 of 12 design and dynamic control of the simplified separation process for MMA by using a one-column flowsheet with a middle decanter, which can cut operating costs by 35.9% compared to the industrial three-column design. Large disturbances of the feed composition can be effectively controlled [15]. Chang et al. studied an alternative design for separating mixtures (including methyl methacrylate, methanol, and water) using a distillation column, a stripper and a decanter. Compared with the traditional design process, the operating cost of during this improved design significantly reduced to 25.9%. In addition, based on open/closed-loop sensitivity testing, the overall design turns out to ensures the product of MMA with a high degree of purification [16]. The azeotropic distillation and ionic liquid eco-environmental separation of methacrolein (MAL) was investigated by Yan et al. to obtain MMA, and results indicated that used green process had significant economic and green-degree advantages [14]. Compared with related reports, C 4 -IDMM has gradually been regarded as a promising green technique, due to the low-cost equipment, short reaction path, and sufficient raw materials, and so on [12,13,17], though there are no large-scale uses in industry. However, it is still a challenge to develop the production process of MMA based on C 4 -IDMM economically. The method used in our study is based on the improved direct methylation of isobutylene method proposed by the Asahi Kasei Corporation. There is no MAA step during this process, which effectively avoids side reactions such as MAA polymerization, simplifies the process flow, and reduces energy consumption, thereby greatly reducing operating costs and investment costs and making it more competitive.

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Section: Thermodynamic Methods Determinationmentioning

confidence: 99%

Design and Optimization of a Process for the Production of Methyl Methacrylate via Direct Methylation

et al. 2019

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“…Plant-wide process modelling of plasma-assisted processes at large scale can be used as a tool to (1) identify challenges arising from the integration of plasma reactors with existing downstream processing systems and cost drivers that should be further optimized, and (2) estimate total energy requirements. Nonetheless, works in this field are rather limited and are not relevant to ethylene production [13][14][15][16].…”

Section: Introductionmentioning

confidence: 99%

Process Modeling and Evaluation of Plasma-Assisted Ethylene Production from Methane

2019

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The electrification of the petrochemical industry, imposed by the urgent need for decarbonization and driven by the incessant growth of renewable electricity share, necessitates electricity-driven technologies for efficient conversion of fossil fuels to chemicals. Non-thermal plasma reactor systems that successfully perform in lab scale are investigated for this purpose. However, the feasibility of such electrified processes at industrial scale is still questionable. In this context, two process alternatives for ethylene production via plasma-assisted non-oxidative methane coupling have conceptually been designed based on previous work of our group namely, a direct plasma-assisted methane-to-ethylene process (one-step process) and a hybrid plasma-catalytic methane-to-ethylene process (two-step process). Both processes are simulated in the Aspen Plus V10 process simulator and also consider the technical limitations of a real industrial environment. The economically favorable operating window (range of operating conditions at which the target product purity is met at minimum utility cost) is defined via sensitivity analysis. Preliminary results reveal that the hybrid plasma-catalytic process requires 21% less electricity than the direct one, while the electric power consumed for the plasma-assisted reaction is the major cost driver in both processes, accounting for ~75% of the total electric power demand. Finally, plasma-assisted processes are not economically viable at present. However, future decrease in electricity prices due to renewable electricity production increase can radically affect process economics. Given that a break-even electricity price of 35 USD/MWh (without considering the capital cost) is calculated for the two-step plasma process and that current electricity prices for some energy intensive industries in certain countries can be as low as 50 USD/MWh, the plasma-assisted processes may become economically viable in the future.

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“…Generally, this process requires high temperatures and operating pressures. Thorough process modelling studies have been performed for plasma dry reforming 17 and plasma non-oxidative methane coupling, 18 which determined that the main operating cost comes from the electricity usage, and that the plasma process could compete with the thermo-catalytic one at the break-even electricity price of 35 $/MWh, which might be the case in the forthcoming times as renewable energy is developed further. Significant yields have been obtained even at atmospheric pressure for syngas production via methane reforming 15,16 ; however, the demand for alternative methods for the reaction operation at lower (ambient) temperatures is increasing.…”

Section: Introductionmentioning

confidence: 99%

“…A promising alternative route, enabling room temperature methane oxidation to value-added chemicals at atmospheric pressure, is the use of atmospheric pressure nonequilibrium plasmas, where high energy electrons can activate methane and induce chemical reactions. Thorough process modelling studies have been performed for plasma dry reforming 17 and plasma non-oxidative methane coupling, 18 which determined that the main operating cost comes from the electricity usage, and that the plasma process could compete with the thermo-catalytic one at the break-even electricity price of 35 $/MWh, which might be the case in the forthcoming times as renewable energy is developed further. Energy efficiency aside, the main advantage of using plasma is the room temperature operation, which prevents some thermodynamically driven reactions at higher temperatures, such as organic product oxidation.…”

Section: Introductionmentioning

confidence: 99%

Plasma‐activated methane partial oxidation reaction to oxygenate platform chemicals over Fe, Mo, Pd and zeolite catalysts

et al. 2019

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Summary Natural gas from stranded sources is being predominantly flared, and there is a growing demand for new technologies for its utilisation, where electrification, flexibility, and modularity play an important role. Plasma‐activated methane partial oxidation reaction was studied in a designed dielectric barrier discharge ionisation reactor unit, producing value‐added platform chemicals, namely, methanol, formaldehyde, intermediate formic acid, acetic acid, and paraformaldehyde at ambient temperature and atmospheric pressure. The effects of various process parameters, such as voltage, total convertible gas flow rate, and reagent ratio relationship, were considered. In addition, coupling of the following catalytic materials with plasma was examined: alumina (Al2O3), chabazite, ferrierite, microporous beta zeolite, silica (SiO2) glass beads, ZSM‐5 (MFI), Fe on H‐ZSM‐5 and Al2O3, Mo on H‐ZSM‐5, TiO2 and SiO2, and Pd on Al2O3. In the liquid product, 21.5% CH3OH, 20.4% CH2O, 0.3% HCOOH, and 2.4% CH3COOH were measured when using pure plasma, and a maximum aggregate yield of the organic oxygenate compounds of 5.21 mol.% was achieved. The usage of shaped silicate surface increased the selectivity towards synthesised oxygen‐containing structures, while the application of alumino‐silicate mixture constituents reduced it. It was determined that elementary covalently bonded carbon was formed inside pores when pure zeolites were used. Fe‐ and Pd‐based heterogeneous catalysts favoured the complete exothermic combustion of CH4 feedstock reactant species, and the liquid product consisted only of water in the Pd‐ case. The utilisation of Mo/H‐ZSM‐5 resulted in a 46% increased yield of formalin. A mechanism for the role of Mo was proposed, where Mo oxidises methanol to formaldehyde and the metal is reoxidised in plasma.

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Investigating the Plasma-Assisted and Thermal Catalytic Dry Methane Reforming for Syngas Production: Process Design, Simulation and Evaluation

Cited by 28 publications

References 73 publications

Design and Optimization of a Process for the Production of Methyl Methacrylate via Direct Methylation

Design and Optimization of a Process for the Production of Methyl Methacrylate via Direct Methylation

Process Modeling and Evaluation of Plasma-Assisted Ethylene Production from Methane

Plasma‐activated methane partial oxidation reaction to oxygenate platform chemicals over Fe, Mo, Pd and zeolite catalysts

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