Methanation of CO<sub>2</sub> Using MIL-53-Based Catalysts: Ni/MIL-53–Al<sub>2</sub>O<sub>3</sub> versus Ni/MIL-53

MIL-53 and the MIL-53–Al<sub>2</sub>O<sub>3</sub> composite synthesized by a solvothermal procedure, with water as the only solvent besides CrCl<sub>3</sub> and benzene-1,4-dicarboxylic acid (BDC), were used as catalytic supports to obtain the novel MIL-53-based c...

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Autores principales: Oana Grad, Gabriela Blanita, Mihaela D. Lazar, Maria Mihet
Formato: article
Lenguaje:EN
Publicado: MDPI AG 2021
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Acceso en línea:https://doaj.org/article/b4724aab9c6f45c2bf13fa393d63f258
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Sumario:MIL-53 and the MIL-53–Al<sub>2</sub>O<sub>3</sub> composite synthesized by a solvothermal procedure, with water as the only solvent besides CrCl<sub>3</sub> and benzene-1,4-dicarboxylic acid (BDC), were used as catalytic supports to obtain the novel MIL-53-based catalysts Ni(10 wt.%)/MIL-53 and Ni(10 wt.%)/MIL-53–Al<sub>2</sub>O<sub>3</sub>. Ni nanoparticle deposition by an adapted double-solvent method leads to the uniform distribution of metallic particles, both smaller (≤10 nm) and larger ones (10–30 nm). MIL-53–Al<sub>2</sub>O<sub>3</sub> and Ni/MIL-53–Al<sub>2</sub>O<sub>3</sub> show superior thermal stability to MIL-53 and Ni/MIL-53, while MIL-53–Al<sub>2</sub>O<sub>3</sub> samples combine the features of both MIL-53 and alumina in terms of porosity. The investigation of temperature’s effect on the catalytic performance in the methanation process (CO<sub>2</sub>:H<sub>2</sub> = 1:5.2, GHSV = 4650 h<sup>−1</sup>) revealed that Ni/MIL-53 is more active at temperatures below 300 °C, and Ni/MIL-53–Al<sub>2</sub>O<sub>3</sub> above 300 °C. Both catalysts show maximum CO<sub>2</sub> conversion at 350 °C: 75.5% for Ni/MIL-53 (methane selectivity of 93%) and 88.8% for Ni/MIL-53–Al<sub>2</sub>O<sub>3</sub> (methane selectivity of 98%). Stability tests performed at 280 °C prove that Ni/MIL-53–Al<sub>2</sub>O<sub>3</sub> is a possible candidate for the CO<sub>2</sub> methanation process due to its high CO<sub>2</sub> conversion and CH<sub>4</sub> selectivity, corroborated by the preservation of the structure and crystallinity of MIL-53 after prolonged exposure in the reaction medium.