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One-step direct conversion of methane to methanol with water in non-thermal plasma.

ABSTRACT: Achieving methane-to-methanol is challenging under mild conditions. In this study, methanol is synthesized by one-step direction conversion of CH₄ with H₂O at room temperature under atmospheric pressure in non-thermal plasma (NTP). This route is characterized by the use of methane and liquid water as the reactants, which enables the transfer of the methanol product to the liquid phase in time to inhibit its further decomposition and conversion. Therefore, the obtained product is free of carbon dioxide. The reaction products include gas and liquid-phase hydrocarbons, CO, CH₃OH, and C₂H₅OH. The combination of plasma and semiconductor materials increases the production rate of methanol. In addition, the addition of Ar or He considerably increases the production rate and selectivity of methanol. The highest production rate of methanol and selectivity in liquid phase can reach 56.7 mmol g_cat^-1 h^-1 and 93%, respectively. Compared with the absence of a catalyst and added gas, a more than 5-fold increase in the methanol production rate is achieved.

SUBMITTER: Bi W

PROVIDER: S-EPMC9814404 | biostudies-literature | 2022 Oct

REPOSITORIES: biostudies-literature

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One-step direct conversion of methane to methanol with water in non-thermal plasma.

Bi Wenfei W Tang Yu Y Li Xuemei X Dai Chengyi C Song Chunshan C Guo Xinwen X Ma Xiaoxun X

Communications chemistry 20221010 1

Achieving methane-to-methanol is challenging under mild conditions. In this study, methanol is synthesized by one-step direction conversion of CH<sub>4</sub> with H<sub>2</sub>O at room temperature under atmospheric pressure in non-thermal plasma (NTP). This route is characterized by the use of methane and liquid water as the reactants, which enables the transfer of the methanol product to the liquid phase in time to inhibit its further decomposition and conversion. Therefore, the obtained produ ...[more]

PMID: 36698023

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Project description:The effect of the phase transformation of a FePO4 catalyst material from the tridymite-like (tdm) FePO4 to the α-domain (α-Fe3(P2O7)2) during the direct selective oxidation of methane to methanol was studied using oxidant species O2, H2O and N2O. The main reaction products were CH3OH, carbon dioxide and carbon monoxide, whereas formaldehyde was produced in rather minute amounts. Results showed that the single-step non-syngas activation of CH4 to oxygenate(s) on a solid FePO4 phase-specific catalyst was influenced by the nature of the oxidizer used for the CH4 turnover. Fresh and activated FePO4 powder samples and their modified physicochemical surface and bulk properties, which affected the conversion and selectivity in the partial oxidation (POX) mechanism of CH4, were investigated. Temperature-programmed re-oxidation (TPRO) profiles indicated that the type of moieties utilised in the procedures, determined the re-oxidizing pathway of the reduced multiphase FePO4 system. Mössbauer spectroscopy measurements along with X-ray diffraction (XRD) examination of neat, hydrogenated and spent catalytic compounds, demonstrated a variation of the phosphate into a mixture of crystallites, which depended on operating process conditions (for example time-on-stream). The Mössbauer spectra revealed the change of the initial ferric orthophosphate, FePO4 (tdm), to the divalent metal form, iron(ii) pyrophosphate (Fe2P2O7); thereafter, reactivity was governed by the interaction (strength) with individual oxidizing agents. The Fe3+ ↔ Fe2+ chemical redox cycle can play a key mechanistic role in tailored multistep design, while the advantage of iron-based heterogeneous catalysis primarily lies in being inexpensive and comprising non-critical raw resources. When compared to the other catalysts reported in the literature, the FePO4-tdm phase catalysts showed in this work exhibited a high activity towards methanol i.e., 12.3 × 10-3 μmolMeOH gcat h-1 using N2O as an oxidant. This catalyst also showed a high activity with O2 as an oxidant (5.3 × 10-3 μmolMeOH gcat h-1). Further investigations will include continuous reactor unit engineering optimisation.

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One-step direct conversion of methane to methanol with water in non-thermal plasma.

Publications

One-step direct conversion of methane to methanol with water in non-thermal plasma.

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