Enhanced CO2 conversion by frosted dielectric surface with ZrO2 coating in a dielectric barrier discharge reactor

Ding, Wanyan; Xia, Mengyu; Shen, Chenyang; Wang, Yaolin; Zhang, Zhitao; Tu, Xin; Liu, Changjun

doi:10.1016/j.jcou.2022.102045

Cited by 20 publications

(10 citation statements)

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“…N–In 2 O 3 was prepared using a plasma-intensified nitrogen doping technology, with which a dielectric barrier discharge (DBD) plasma was applied. , DBD plasma is a conventional plasma phenomenon, which can be operated at room temperature and atmospheric pressure. Before the plasma nitrogen doping, the pristine In 2 O 3 was placed into a discharge chamber.…”

Section: Methodsmentioning

confidence: 99%

“…The DBD plasma was initiated for nitrogen doping for 30 min. More details on the setup and operation of the DBD plasma have been given in our previous works. , …”

Section: Methodsmentioning

confidence: 99%

“…More details on the setup and operation of the DBD plasma have been given in our previous works. 39,40 The catalyst characterization shows that the particle size of N−In 2 O 3 is larger than that of the pristine In 2 O 3 (Figure S1). Pure argon was used as the DBD plasma-generating gas to treat the pristine In 2 O 3 under the same conditions as those used for the preparation of N−In 2 O 3 , in order to study the effect of particle size on the catalytic performance.…”

Section: Methodsmentioning

confidence: 99%

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Enhanced Surface Charge Localization Over Nitrogen-Doped In₂O₃ for CO₂ Hydrogenation to Methanol with Improved Stability

et al. 2023

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Indium oxide (In 2 O 3 ) is active and promising for selective hydrogenation of CO 2 to methanol. However, it suffers from over-reduction at elevated temperatures, causing deactivation. Herein, a nitrogen-doped In 2 O 3 (N−In 2 O 3 ) catalyst was prepared using a plasma-intensified nitrogen-doping technology. It is confirmed that nitrogen doping is effective for the stabilization of In 2 O 3 . The doped nitrogen enhances the surface charge localization, which inhibits the over-reduction on the oxide surface and limits the generation of excessive surface oxygen vacancies. The doped nitrogen also serves as the active site, synergistically with surface oxygen vacancy, which leads to an enhanced dissociation of CO 2 to adsorbed CO* intermediates. The electron-rich nitrogen causes a strong adsorption of CO on N−In 2 O 3 and inhibits the formation of free CO. A significantly improved methanol selectivity with a higher turnover frequency (TOF) is thus achieved on N− In 2 O 3 , compared to the un-doped In 2 O 3 . For example, at 21,000 cm 3 h −1 g cat −1 , 300 °C, and 5 MPa, the TOF of N−In 2 O 3 reaches 37.0 h −1 with methanol selectivity of 75.1%, while the TOF of the un-doped In 2 O 3 is only 16.0 h −1 with methanol selectivity of 62.3%. Different from pristine In 2 O 3 , N−In 2 O 3 takes the CO hydrogenation route for CO 2 hydrogenation to methanol. This explains the reason why the N−In 2 O 3 catalyst possesses improved selectivity for CO 2 hydrogenation to methanol.

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Section: Methodsmentioning

confidence: 99%

“…The DBD plasma was initiated for nitrogen doping for 30 min. More details on the setup and operation of the DBD plasma have been given in our previous works. , …”

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

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Enhanced Surface Charge Localization Over Nitrogen-Doped In₂O₃ for CO₂ Hydrogenation to Methanol with Improved Stability

et al. 2023

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“…), revealing propane to be the most prone to degradation, with depletion efficiencies ranging between 2 and 7.5 g/kWh. Cold plasma was recently applied to convert CO 2 to CO and O 2 , responding to the problem of carbon dioxide fixation/exploitation (Ding et al, 2022). Ding and co-workers proposed a flow protocol were ZrO 2 -coated frosted DBD plasma was exploited giving an overall conversion of 21.7%, under a flow rate of 10 ml/min, by exerting 14.5 W of discharge power and a max.…”

Section: Cold Plasmamentioning

confidence: 99%

Process intensification in continuous flow organic synthesis with enabling and hybrid technologies

et al. 2022

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Industrial organic synthesis is time and energy consuming, and generates substantial waste. Traditional conductive heating and mixing in batch reactors is no longer competitive with continuous-flow synthetic methods and enabling technologies that can strongly promote reaction kinetics. These advances lead to faster and simplified downstream processes with easier workup, purification and process scale-up. In the current Industry 4.0 revolution, new advances that are based on cyber-physical systems and artificial intelligence will be able to optimize and invigorate synthetic processes by connecting cascade reactors with continuous in-line monitoring and even predict solutions in case of unforeseen events. Alternative energy sources, such as dielectric and ohmic heating, ultrasound, hydrodynamic cavitation, reactive extruders and plasma have revolutionized standard procedures. So-called hybrid or hyphenated techniques, where the combination of two different energy sources often generates synergistic effects, are also worthy of mention. Herein, we report our consolidated experience of all of these alternative techniques.

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“…Several different plasma systems have been applied to CO 2 dissociation studies since then, based on DBD 7 – 13 , glow discharges 6 , 14 , 15 , microwaves 4 , gliding and rotating arcs 11 , 16 – 20 both for direct CO 2 disintegration and towards its valorization via methanation 11 , 21 , 22 , dry reforming 23 – 25 and for the production of liquids 26 when catalytic systems are added to the discharge region. To our best knowledge, the highest efficiency reported to this day is up to 43%, for a glow discharge (GD) (in fact a rotating arc) system 7 and 50% for a large microwave discharge operating at 4 kW 27 However, none of these studies involved the use of high power (kW), water cooled DBDs.…”

Section: Introductionmentioning

confidence: 99%

A water cooled, high power, dielectric barrier discharge reactor for CO2 plasma dissociation and valorization studies

Lisi

Laverdura

Chierchia

et al. 2023

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Aiming at the energy efficient use and valorization of carbon dioxide in the framework of decarbonization studies and hydrogen research, a novel dielectric barrier discharge (DBD) reactor has been designed, constructed and developed. This test rig with water cooled electrodes is capable of a plasma power tunable in a wide range from 20W to 2 kW per unit. The reactor was designed to be ready for catalysts and membrane integration aiming at a broad range plasma conditions and processes, including low to moderate high pressures (0.05–2 bar). In this paper, preliminary studies on the highly endothermic dissociation of CO2, into O2 and CO, in a pure, inert, and noble gas mixture flow are presented. These initial experiments were performed in a geometry with a 3 mm plasma gap in a chamber volume of 40cm3, where the process pressure was varied from few 200 mbar to 1 bar, using pure CO2, and diluted in N2. Initial results confirmed the well-known trade-off between conversion rate (up to 60%) and energy efficiency (up to 35%) into the dissociation products, as measured downstream of the reactor system. Improving conversion rate, energy efficiency and the trade-off curve can be further accomplished by tuning the plasma operating parameters (e.g. the gas flow and system geometry). It was found that the combination of a high-power, water-cooled plasma reactor, together with electronic and waveform diagnostic, optical emission and mass spectroscopies provides a convenient experimental framework for studies on the chemical storage of fast electric power transients and surges.

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Enhanced CO2 conversion by frosted dielectric surface with ZrO2 coating in a dielectric barrier discharge reactor

Cited by 20 publications

References 50 publications

Enhanced Surface Charge Localization Over Nitrogen-Doped In₂O₃ for CO₂ Hydrogenation to Methanol with Improved Stability

Enhanced Surface Charge Localization Over Nitrogen-Doped In₂O₃ for CO₂ Hydrogenation to Methanol with Improved Stability

Process intensification in continuous flow organic synthesis with enabling and hybrid technologies

A water cooled, high power, dielectric barrier discharge reactor for CO2 plasma dissociation and valorization studies

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Enhanced CO2 conversion by frosted dielectric surface with ZrO2 coating in a dielectric barrier discharge reactor

Cited by 20 publications

References 50 publications

Enhanced Surface Charge Localization Over Nitrogen-Doped In2O3 for CO2 Hydrogenation to Methanol with Improved Stability

Enhanced Surface Charge Localization Over Nitrogen-Doped In2O3 for CO2 Hydrogenation to Methanol with Improved Stability

Process intensification in continuous flow organic synthesis with enabling and hybrid technologies

A water cooled, high power, dielectric barrier discharge reactor for CO2 plasma dissociation and valorization studies

Contact Info

Product

Resources

About

Enhanced Surface Charge Localization Over Nitrogen-Doped In₂O₃ for CO₂ Hydrogenation to Methanol with Improved Stability

Enhanced Surface Charge Localization Over Nitrogen-Doped In₂O₃ for CO₂ Hydrogenation to Methanol with Improved Stability