Ignition of CO2 methanation using DBD-plasma catalysis in an adiabatic reactor

Biset‐Peiró, Martí; Guilera, Jordi; Andreu, Teresa

doi:10.1016/j.cej.2021.133638

Cited by 8 publications

(6 citation statements)

References 27 publications

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“…Indeed, the extra heat produced by the exothermic process is harvested and exploited in turn as a useful energy source to keep the methanation reaction alive even when its primary external heating source is switched off [36] . Besides the outstanding methanation performance obtained with Ni/UO x catalysts under exceptionally low temperature settings, the study offers a concrete solution to the challenging problem of the extra heat harvesting looking beyond the simple employment of adiabatic reactor schemes [37] . Ni/UO x catalysts have also shown remarkable stability and durability throughout a very long‐term methanation run (>400 h).…”

Section: Introductionmentioning

confidence: 93%

“…[36] Besides the outstanding methanation performance obtained with Ni/UO x catalysts under exceptionally low temperature settings, the study offers a concrete solution to the challenging problem of the extra heat harvesting looking beyond the simple employment of adiabatic reactor schemes. [37] Ni/UO x catalysts have also shown remarkable stability and durability throughout a very long-term methanation run (> 400 h). Evidence for a permanent catalyst modification with the generation of Ni/UO x core-shelllike composites (as the result of an extensive segregation of UO x particles all around larger Ni NPs aggregates) is also provided and discussed.…”

Section: Introductionmentioning

confidence: 99%

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Not Just Another Methanation Catalyst: Depleted Uranium Meets Nickel for a High‐Performing Process Under Autothermal Regime

et al. 2022

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Ni-based catalysts prepared through impregnation of depleted uranium oxides (DU) have successfully been employed as highly efficient, selective, and durable systems for CO 2 hydrogenation to substituted natural gas (SNG; CH 4 ) under an autothermal regime. The thermo-physical properties of DU and the unique electronic structure of f-block metal-oxides combined with a nickel active phase, generated an ideal catalytic assembly for turning waste energy back into useful energy for catalysis. In particular, Ni/UO x stood out for the capacity of DU matrix to control the extra heat (hot-spots) generated at its surface by the highly exothermic methanation process. At odds with the benchmark Ni/γ-Al 2 O 3 catalyst, the double action played by DU as a "thermal mass" and "dopant" for the nickel active phase unveiled the unique performance of Ni/UO x composites as CO 2 methanation catalysts. The ability of the weakly radioactive ceramic (UO x ) to harvest waste heat for more useful purposes was demonstrated in practice within a rare example of a highly effective and long-term methanation operated under autothermal regime (i. e., without any external heating source). This finding is an unprecedented example that allows a real stepforward in the intensification of "low-temperature" methanation with an effective reduction of energy wastes. At the same time, the proposed catalytic technology can be regarded as an original approach to recycle and bring to a second life a lesssevere nuclear by-product (DU), providing a valuable alternative to its more costly long-term storage or controlled disposal.

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Section: Introductionmentioning

confidence: 93%

Section: Introductionmentioning

confidence: 99%

Not Just Another Methanation Catalyst: Depleted Uranium Meets Nickel for a High‐Performing Process Under Autothermal Regime

et al. 2022

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“…At the same time, this also confirms the advantages of using an insulated reactor (collection of plasmaderived heat using a tube furnace). 39 This may involve contributions from partial pore volume characteristics, but the correlation with surface area is relatively small. For instance, SiO 2 and MCM-41 have a 6.4-fold difference in the surface area, but they exhibit almost the same ammonia synthesis concentration (SiO 2 : 9375 ppm, MCM-41:9533 ppm).…”

Section: Materials Activitymentioning

confidence: 99%

Unlocking Efficient Synergistic Plasma-Catalyst Ammonia Synthesis: System Optimization and Catalyst Support Screening

Chen,

Tang,

et al. 2024

Energy Fuels

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Plasma catalysis for ammonia synthesis technology exhibits significant development potential, and improving the synergistic interaction between plasma and catalyst is a challenging research focus. However, current research focuses on efficient catalyst formulation design, but studies on catalyst support material screening and reactor performance optimization are lacking. Therefore, this study first enhanced the ammonia synthesis capability of the reactor and found that the 5 cm ground electrode and center plasma catalysis (CPC) coupling were the optimal system configurations. Support screening tests showed that higher dielectric properties and highly ordered interconnecting pores are crucial to achieving high ammonia concentration production. The SBA-15 (best material) filled system showed the highest reduced electric field (122.97 Td), with a more significant number of high-energy electrons and an average electron energy of up to 3.93 eV. Possible enhanced mechanisms for ammonia synthesis on SBA-15 include: (1) promoting the excitation dissociation process of feed gas in the gas phase and the activation process on the material surface and (2) using ordered tubular channels to suppress the occurrence of plasma-induced reverse reactions. By adjusting the flow rate, ammonia concentration as high as 11737 ppm was achieved, 4.58 times higher than the empty tube. The highest achieved synthesis rate was 5337 μmol/gcat/h, and the energy yield was 1.04 gNH3 /kWh. Additionally, the study indicated that a nitrogen-rich environment is more beneficial for the progression of the reaction, with the optimal N2:H2 molar ratio being 2:1. This work highlights the necessity and significance of optimizing the reaction system, including (1) system configuration, (2) catalyst support material, and (3) operating parameter. Especially, it provides new insights into the design of catalysts in a plasma environment.

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“…All of this can be accomplished while maintaining a low background temperature, which is critical because decomposition temperatures for known pentazolate compounds are typically 100 °C or less at ambient pressure. This unique reaction environment in nonequilibrium plasmas has been used to activate relatively inert molecules to perform chemistry at low temperature, for example N 2 , − CO 2 , − and CH 4 ,− can all be made to react at relatively low background temperature and pressures from vacuum to near ambient.…”

Section: Introductionmentioning

confidence: 99%

Polynitrogen High Energy Density Materials Synthesized by Nonequilibrium Plasma

Thimsen

2023

J. Phys. Chem. C

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Metal pentazolate compounds that contain 5-nitrogen singly charged anion rings are an interesting class of materials from a thermodynamics perspective. These compounds are believed to be equilibrium phases only at extremely high pressures, and thus, they constitute exotic states of matter at ambient pressure and temperature. Moreover, the energy released by these pentazolate compounds upon relaxation to the equilibrium state at ambient conditions is in the range 1 to 10 MJ per kg, rivaling that of combustion reactions. The synthesis of pentazolates is not an easy task, and there are only two known methods, each of which has significant challenges. The development of new scalable synthesis routes could enable the production of these exotic materials in sufficient quantity to explore their properties more widely beyond the context of explosives and propellants. In this Perspective, it is argued that nonequilibrium plasma is a promising reaction medium for the synthesis of metal pentazolate compounds, for example from the corresponding metal azide and N 2 gas activated by the discharge at low background temperature.

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Ignition of CO2 methanation using DBD-plasma catalysis in an adiabatic reactor

Cited by 8 publications

References 27 publications

Not Just Another Methanation Catalyst: Depleted Uranium Meets Nickel for a High‐Performing Process Under Autothermal Regime

Not Just Another Methanation Catalyst: Depleted Uranium Meets Nickel for a High‐Performing Process Under Autothermal Regime

Unlocking Efficient Synergistic Plasma-Catalyst Ammonia Synthesis: System Optimization and Catalyst Support Screening

Polynitrogen High Energy Density Materials Synthesized by Nonequilibrium Plasma

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