Revealing the active sites of the structured Ni-based catalysts for one-step CO2/CH4 conversion into oxygenates by plasma-catalysis

Li, Jiangwei; Dou, Liguang; Gao, Yuan; Hei, Xueting; Ye, Feng; Shao, Tao

doi:10.1016/j.jcou.2021.101675

Cited by 33 publications

(8 citation statements)

References 59 publications

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“…Mixtures of methane and CO 2 tend to produce more higher hydrocarbons and a more complex mixture of liquid C 1 and C 2 oxygenates , and appear to require even more electrical power, but the potential application to biogas (in particular) remains intriguing. Clearly, for both CH 4 /O 2 and CH 4 /CO 2 , there is a very complex interaction between the gaseous “plasma phase” and reactor/electrode/catalyst surfaces, including adsorbed species, where bulk catalysts and surfaces affect the physical nature of the discharge and the discharge affects the chemistry at the surfaces.…”

Section: Background Chemistrymentioning

confidence: 99%

Methane Oxidation to Methanol

et al. 2022

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The direct transformation of methane to methanol remains a significant challenge for operation at a larger scale. Central to this challenge is the low reactivity of methane at conditions that can facilitate product recovery. This review discusses the issue through examination of several promising routes to methanol and an evaluation of performance targets that are required to develop the process at scale. We explore the methods currently used, the emergence of active heterogeneous catalysts and their design and reaction mechanisms and provide a critical perspective on future operation. Initial experiments are discussed where identification of gas phase radical chemistry limited further development by this approach. Subsequently, a new class of catalytic materials based on natural systems such as iron or copper containing zeolites were explored at milder conditions. The key issues of these technologies are low methane conversion and often significant overoxidation of products. Despite this, interest remains high in this reaction and the wider appeal of an effective route to key products from C–H activation, particularly with the need to transition to net carbon zero with new routes from renewable methane sources is exciting.

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Section: Background Chemistrymentioning

confidence: 99%

Methane Oxidation to Methanol

et al. 2022

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“…[1,2] Recently, researchers have paid more attention to CO 2 conversion, which is a promising method to dispose of it using H sources such as H 2 , [3,4] H 2 O, [5] and/or CH 4 . [6][7][8][9] However, the conventional dry reforming of CH 4 is subject to higher thermodynamic limitations. Therefore, the hydrogenation of CO 2 is a promising approach to dispose of it with a source to produce CO, CH 4 , CH 3 OH, and lower olefins (C2-C4).…”

Section: Introductionmentioning

confidence: 99%

Efficient CH₃OH formation on H₂/Ar plasma‐treated CoO sites for CO₂ + H₂ + H₂O DBD system

Pan

Dou

et al. 2023

Plasma Processes & Polymers

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Packing heterogeneous catalysts to achieve a better plasma–catalyst synergy is critical to promoting CO2 conversion into high‐value chemicals. Herein, a series of CoO‐based catalysts were synthesized, and the treated H2/Ar–CoO possessed the highest CH3OH selectivity (39.6%) in the CO2 + H2 + H2O system, about four times higher than the initial CoO (10.0%). Systemic characterizations showed that H2/Ar plasma treatment significantly increased the oxygen vacancy (Ov) concentration of H2/Ar–CoO by Ar+ bombardment and synchronous H reduction. Considering the key role of CH3O on CH3OH generation upon kinetic simulations, we proposed that the Ov in H2/Ar–CoO could accelerate the CH3O/OH adsorption and further recombine with H/CH3, in which the H2O provided abundant OH/H radicals via electron‐impact process. This study highlighted the importance of using H2O with Ov‐rich catalysts for plasma‐enabled CH3OH synthesis.

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“…[ 22 ] Li et al investigated the plasma‐enabled CH 4 dry reforming over the various Ni‐based catalysts, successfully realized conversion from CH 4 to CH 3 OH and CH 3 COOH, revealing the facilitation of OH radicals. [ 23 ] On the other hand, most of research on NTP‐driven CH 3 OH conversion mainly focuses on the hydrogen production, [ 24 ] such as Lü et al designed a gliding arc (GA) discharge plasma to drive hydrogen generation from CH 3 OH, which achieved the conversion of CH 3 OH (51%–81.7%) with a constant H 2 selectivity (~46%). [ 25 ] Moreover, Zhang et al also reported the hydrogen production from CH 3 OH decomposition by GA discharge plasma, which reached a maximum CH 3 OH conversion of 87.1%, providing an promising method for industrial hydrogen production.…”

Section: Introductionmentioning

confidence: 99%

Parametric investigations on plasma‐activated conversion of CH₄–CH₃OH to C2–C4 alcohols by nanosecond pulsed discharge

Gao

Dou

et al. 2022

Plasma Processes & Polymers

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Revealing the active sites of the structured Ni-based catalysts for one-step CO2/CH4 conversion into oxygenates by plasma-catalysis

Cited by 33 publications

References 59 publications

Methane Oxidation to Methanol

Methane Oxidation to Methanol

Efficient CH₃OH formation on H₂/Ar plasma‐treated CoO sites for CO₂ + H₂ + H₂O DBD system

Parametric investigations on plasma‐activated conversion of CH₄–CH₃OH to C2–C4 alcohols by nanosecond pulsed discharge

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Revealing the active sites of the structured Ni-based catalysts for one-step CO2/CH4 conversion into oxygenates by plasma-catalysis

Cited by 33 publications

References 59 publications

Methane Oxidation to Methanol

Methane Oxidation to Methanol

Efficient CH3OH formation on H2/Ar plasma‐treated CoO sites for CO2 + H2 + H2O DBD system

Parametric investigations on plasma‐activated conversion of CH4–CH3OH to C2–C4 alcohols by nanosecond pulsed discharge

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Product

Resources

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Efficient CH₃OH formation on H₂/Ar plasma‐treated CoO sites for CO₂ + H₂ + H₂O DBD system

Parametric investigations on plasma‐activated conversion of CH₄–CH₃OH to C2–C4 alcohols by nanosecond pulsed discharge