Dataset Information

One-Step Reforming of CO₂ and CH₄ into High-Value Liquid Chemicals and Fuels at Room Temperature by Plasma-Driven Catalysis.

ABSTRACT: The conversion of CO₂ with CH₄ into liquid fuels and chemicals in a single-step catalytic process that bypasses the production of syngas remains a challenge. In this study, liquid fuels and chemicals (e.g., acetic acid, methanol, ethanol, and formaldehyde) were synthesized in a one-step process from CO₂ and CH₄ at room temperature (30 °C) and atmospheric pressure for the first time by using a novel plasma reactor with a water electrode. The total selectivity to oxygenates was approximately 50-60 %, with acetic acid being the major component at 40.2 % selectivity, the highest value reported for acetic acid thus far. Interestingly, the direct plasma synthesis of acetic acid from CH₄ and CO₂ is an ideal reaction with 100 % atom economy, but it is almost impossible by thermal catalysis owing to the significant thermodynamic barrier. The combination of plasma and catalyst in this process shows great potential for manipulating the distribution of liquid chemical products in a given process.

SUBMITTER: Wang L

PROVIDER: S-EPMC5656906 | biostudies-literature | 2017 Oct

REPOSITORIES: biostudies-literature

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Publications

One-Step Reforming of CO2 and CH4 into High-Value Liquid Chemicals and Fuels at Room Temperature by Plasma-Driven Catalysis.

Wang Li L Yi Yanhui Y Wu Chunfei C Guo Hongchen H Tu Xin X

Angewandte Chemie (International ed. in English) 20170919 44

The conversion of CO2 with CH4 into liquid fuels and chemicals in a single-step catalytic process that bypasses the production of syngas remains a challenge. In this study, liquid fuels and chemicals (e.g., acetic acid, methanol, ethanol, and formaldehyde) were synthesized in a one-step process from CO2 and CH4 at room temperature (30 °C) and atmospheric pressure for the first time by using a novel plasma reactor with a water electrode. The total selec ...[more]

PMID: 28842938

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Project description:The chemical looping reforming of methane using an SrFeO3 oxygen carrier to produce synthesis gas from solar energy was experimentally investigated and validated. High-temperature solar heat was used to provide the reaction enthalpy, and therefore the methane feedstock was entirely dedicated to producing syngas. The two-step isothermal process encompassed partial perovskite reduction with methane (partial oxidation of CH4) and exothermic oxidation of SrFeO3-δ with CO2 or H2O splitting under the same operating temperature. The oxygen carrier material was shaped in the form of a reticulated porous foam structure for enhancing heat and mass transfer, and it was cycled in a solar-heated tubular reactor under different operating parameters (temperature: 950-1050 °C, methane mole fraction: 5-30%, and type of oxidant gas: H2O vs. CO2). This study aimed to assess the fuel production capacity of the two-step process and to demonstrate the potential of using strontium ferrite perovskite during solar cycling for the first time. The maximum H2 and CO production rates during CH4-induced reduction were 70 and 25 mL/min at 1000 °C and 15% CH4 mole fraction. The increase in both the cycle temperature and the methane mole fraction promoted the reduction step, thereby enhancing syngas yields up to 569 mL/g during reduction at 1000 °C under 30% CH4 (778 mL/g including both cycle steps), and thus outperforming the performance of the benchmark ceria material. In contrast, the oxidation step was not significantly affected by the experimental conditions and the material's redox performance was weakly dependent on the nature of the oxidizing gas. The syngas yield remained above 200 mL/g during the oxidation step either with H2O or CO2. Twelve successive redox cycles with stable patterns in the syngas production yields validated material stability. Combining concentrated solar energy and chemical looping reforming was shown to be a promising and sustainable pathway toward carbon-neutral solar fuels.

Dataset Information

One-Step Reforming of CO₂ and CH₄ into High-Value Liquid Chemicals and Fuels at Room Temperature by Plasma-Driven Catalysis.

Publications

One-Step Reforming of CO<sub>2</sub> and CH<sub>4</sub> into High-Value Liquid Chemicals and Fuels at Room Temperature by Plasma-Driven Catalysis.

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