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    Non-oxidative methane conversion in microwave-assisted structured reactors

    Year: 2019

    Journal: Chem. Eng. J., Volume 377, 1-Dec

    Authors: Julian, Ignacio; Ramirez, Heidy; Hueso, Jose L.; Mallada, Reyes; Santamaria, Jesus

    Organizations: European Union's Horizon 2020 Research and Innovation Programme (ADREM project) [680777]

    Country: Florence, ITALY

    Keywords: Microwave-assisted heterogeneous catalysis; Methane non-oxidative coupling; Methane dehydroaromatization; Gas-solid temperature gradient; Microwave selective heating; MoZSM5

    The main problem to be addressed in the valorization of methane under non-oxidative conditions (MNOC) is to reduce or even avoid coke formation. In this work we report the use of microwave-assisted heating for MNOC. We have developed a system able to heat-up a Mo-ZSM5 catalyst coated on silicon carbide monolith that could operate stable for at least 19 h at reaction conditions, 700 degrees C. We demonstrate that under MW-heating the selectivity shifts to C(2)s and benzene. In contrast, the operation under conventional heating (CH) produces more coke and polyaromatics. The selective microwave heating has two effects in this reaction: i) during the activation of the catalyst the formation of the active catalytic species of Mo2C inside the microporous support is different affecting the selectivity and product distribution; ii) a gas-solid temperature gradient is established that prevents the formation of coke from PAHs in the gas phase. The MNOC process under controlled MW heating at high space velocity (3000 mL/g(cat).h) gives a hydrocarbon yield of around 6% with a very low deactivation rate. These results open up new possibilities for process intensification using alternative sources of energy, as is the case of microwaves, for heating structured catalytic reactors.
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