Selective oxidation of CH4 to CH3OH through plasma catalysis: Insights from catalyst characterization and chemical kinetics modelling

Yi, Yanhui; Li, Shangkun; Cui, Zhaolun; Hao, Yingzi; Zhang, Yang; Wang, Li; Liu, Pei; Tu, Xin; Xu, Xiaojun; Guo, Hongchen; Bogaerts, Annemie

doi:10.1016/j.apcatb.2021.120384

Cited by 58 publications

(65 citation statements)

References 60 publications

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“…The experimental results of Yi et al [40] for CO, CO 2 , MeOH, FAc, and FA, and of Larkin et al [18] for H 2 confirm the trends found in the present work. The trends observed by Larkin et al [18] for MeFo and C 2 H 6 and by Bhatnagar and Mallison [16] for EtOH, do not agree with those from our study.…”

Section: Selectivitiessupporting

confidence: 91%

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Investigation of Partial Oxidation of Methane in a Cold Plasma Reactor with Detailed Product Analysis

Müller

Ströfer

Kohns

et al. 2022

Plasma Chem Plasma Process

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Cold plasma is a partially ionized state of matter that unites high reactivity and mild conditions. Therefore, cold plasma reactors are intriguing for reaction engineering. In this work, a laboratory scale dielectric barrier discharge (DBD) cold plasma reactor was designed, set up, and used for studying the influence of the specific energy input (SEI) on the product spectrum of the partial oxidation of methane. In total, 23 experiments were carried out near ambient conditions with a molar reactant ratio of methane to oxygen of 2:1 at SEI between 0.3 and 6.0 J cm−3. The feed also contained argon at a mole fraction of 0.75 mol mol−1. The product stream was split into a fraction that was condensed in a cold trap and the remaining gaseous fraction. The latter was analyzed at-line in a gas chromatograph equipped with a dual column and two carrier gases. The condensed fraction was analyzed by qualitative and quantitative 1H and 13C NMR spectroscopy, Karl Fischer titration, and sodium sulfite titration. In the product stream, 16 components were identified and quantified: acetic acid, acetone, carbon dioxide, carbon monoxide, ethanol, ethane, ethene, ethylene glycol, formaldehyde, formic acid, hydrogen, methanol, methyl acetate, methyl hydroperoxide, methyl formate, and water. A univariant influence of the SEI on the conversions of methane and oxygen and the selectivities to the products was observed. The experimental results provided here are an asset for developing reaction kinetic models of the partial oxidation of methane in DBD plasma reactors.

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Section: Selectivitiessupporting

confidence: 91%

“…Besides the experimental data discussed above, Yi et al [40] report also results from reaction kinetic modeling. For CO, CO 2 , and MeOH, they found similar trends as those observed in the present work, while for FAc the opposite trend was found.…”

Section: Selectivitiesmentioning

confidence: 98%

Investigation of Partial Oxidation of Methane in a Cold Plasma Reactor with Detailed Product Analysis

Müller

Ströfer

Kohns

et al. 2022

Plasma Chem Plasma Process

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“…At the same time, energy efficiency improves from the equivalent of 1.85 kWh mol –1 of methanol to 0.58 kWh mol –1 methanol, which is not far above the water electrolysis based e-methanol figures quoted previously and possibly the most important effect of the catalyst. Similarly, Yi and co-workers report an increase in methane conversion from ∼4% to ∼6% with associated increase in methanol selectivity from 42% to 50% (76% to 81% for total oxygenates) on adding a NiO/γ-Al 2 O 3 material . Energy efficiency again improves very substantially from 1.3 kWh mol –1 methanol to 0.71 kWh mol –1 on addition of the catalyst.…”

Section: Background Chemistrymentioning

confidence: 85%

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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“…In plasma catalytic partial oxidation of methane using oxidants such as air (or O 2 ), H 2 O 2 , and CO 2 have also been explored for methanol synthesis. [44][45][46][47][48] There are several disadvantages associated with this process. The use of air or O 2 as an oxidant results in high selectivity to CO and CO 2 (CO x ).…”

Section: Methanol Formation Via Ntp Catalytic Partial Methane Oxidationmentioning

confidence: 99%

“…In plasma catalytic partial oxidation of methane using oxidants such as air (or O 2 ), H 2 O 2 , and CO 2 have also been explored for methanol synthesis 44–48 . There are several disadvantages associated with this process.…”

Section: Methanol Formation Via Ntp Catalytic Partial Methane Oxidationmentioning

confidence: 99%

The application of nonthermal plasma in methanol synthesis via CO₂ hydrogenation

Farahani

Zeng

Zheng

2022

Energy Science & Engineering

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CH3OH is an energy carrier that can be generated from renewable resources and be used as a fuel in fuel cells and internal combustion engines and a platform chemical for the synthesis of value‐added chemicals or gasoline. Carbon dioxide (CO2) hydrogenation is one of the widely researched methods to generate methanol. The traditional CO2 hydrogenation reaction method (requires high H2 pressure and temperatures) has attracted considerable attention. However, the new emerging field of catalysis referred to as nonthermal plasma (NTP) catalysis has also been developed extensively for methane reforming and CO2 hydrogenation to methane and CO. The plasma‐assisted approach not only presents remarkable advantages, such as room temperature and atmospheric H2 pressure but also has great potential to be powered by renewable electricity in a flexible way since it can be easily switched on/off. In this account, we review the recent articles published on methanol synthesis from CO2 and H2 using NTP. We reviewed and discussed the mechanism of this reaction under NTP, the modification of the reactor configurations, and the rationale behind the catalyst design. In the end, we discussed the advantages and disadvantages of each of these works and the future perspectives of this interesting privileged reaction. We believe this review is of interest to researchers active in sustainable heterogeneous catalysis.

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Selective oxidation of CH4 to CH3OH through plasma catalysis: Insights from catalyst characterization and chemical kinetics modelling

Cited by 58 publications

References 60 publications

Investigation of Partial Oxidation of Methane in a Cold Plasma Reactor with Detailed Product Analysis

Investigation of Partial Oxidation of Methane in a Cold Plasma Reactor with Detailed Product Analysis

Methane Oxidation to Methanol

The application of nonthermal plasma in methanol synthesis via CO₂ hydrogenation

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Selective oxidation of CH4 to CH3OH through plasma catalysis: Insights from catalyst characterization and chemical kinetics modelling

Cited by 58 publications

References 60 publications

Investigation of Partial Oxidation of Methane in a Cold Plasma Reactor with Detailed Product Analysis

Investigation of Partial Oxidation of Methane in a Cold Plasma Reactor with Detailed Product Analysis

Methane Oxidation to Methanol

The application of nonthermal plasma in methanol synthesis via CO2 hydrogenation

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The application of nonthermal plasma in methanol synthesis via CO₂ hydrogenation