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    Item type:Publication,
    Chemical Looping CH4 Reforming Through Isothermal Two-Step Redox Cycling of SrFeO3 Oxygen Carrier in a Tubular Solar Reactor
    (2025-03-01)
    Abanades, Stéphane
    ;
    Wang, Xinhe
    ;
    The chemical looping reforming of methane using an SrFeO<inf>3</inf> 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 CH<inf>4</inf>) and exothermic oxidation of SrFeO<inf>3-δ</inf> with CO<inf>2</inf> or H<inf>2</inf>O 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: H<inf>2</inf>O vs. CO<inf>2</inf>). 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 H<inf>2</inf> and CO production rates during CH<inf>4</inf>-induced reduction were 70 and 25 mL/min at 1000 °C and 15% CH<inf>4</inf> 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% CH<inf>4</inf> (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 H<inf>2</inf>O or CO<inf>2</inf>. 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.
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    Item type:Publication,
    Solar-driven chemical looping reforming of methane over SrFeO3-δ-Ca0.5Mn0.5O nanocomposite foam
    (2022-09-15)
    Wang, Xinhe
    ;
    Abanades, Stéphane
    ;
    ;
    Zhang, Junshe
    ;
    Wei, Jinjia
    Strontium ferrite (SrFeO<inf>3-δ</inf>) is a very attractive oxygen transfer agent for chemical looping reactions and hydrogen-rich syngas generation. Dispersing SrFeO<inf>3</inf> in a medium such as Ca<inf>0.5</inf>Mn<inf>0.5</inf>O could enhance the activity and cyclability. In this study, SrFeO<inf>3-δ</inf>-Ca<inf>0.5</inf>Mn<inf>0.5</inf>O (30 wt% SrFeO<inf>3-δ</inf>) nanocomposite with a reticulated foam structure was explored as the oxygen carrier for chemical looping reforming of methane in a solar tubular reactor. The foam nanocomposite was prepared by a hard-templating method. The performance was investigated at temperatures of 850–1000 °C and methane flowrates of 25–250 STP mL/min, and the oxidative gas was either CO<inf>2</inf> or H<inf>2</inf>O in the oxidation step. In the reduction step of 27 successive redox cycles, the production rate of CO changed marginally and CO yield maintained at about 1.9 mmol/g, even though sintering occurred. The productivity of H<inf>2</inf> decreased first and then tended to be stable at 3.8 mmol/g (i.e., twice the CO yield) as the cycling number increased (the average oxygen storage capacity of the material was ∼1.95 mmol/g). Microscopic and X-ray diffraction investigations suggested that the element distribution pattern and crystalline phase of the foam nanocomposite remained almost unchanged after 27 redox cycles, confirming material stability. The maximum solar-to-fuel efficiency for the foam nanocomposite was 5.68%, which was 21.4% higher than that for the powder nanocomposite. To increase syngas productivity and solar-to-fuel efficiency, it is required to conduct the reforming reaction at high temperatures and methane flowrates. However, the energy upgrade factor will decrease as methane flowrate increases.