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
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Publicado: MDPI AG 2021
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spelling oai:doaj.org-article:b4724aab9c6f45c2bf13fa393d63f2582021-11-25T17:07:00ZMethanation of CO<sub>2</sub> Using MIL-53-Based Catalysts: Ni/MIL-53–Al<sub>2</sub>O<sub>3</sub> versus Ni/MIL-5310.3390/catal111114122073-4344https://doaj.org/article/b4724aab9c6f45c2bf13fa393d63f2582021-11-01T00:00:00Zhttps://www.mdpi.com/2073-4344/11/11/1412https://doaj.org/toc/2073-4344MIL-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.Oana GradGabriela BlanitaMihaela D. LazarMaria MihetMDPI AGarticleMIL-53–Al<sub>2</sub>O<sub>3</sub>Ni/MIL-53 catalystNi/MIL-53–Al<sub>2</sub>O<sub>3</sub> catalystmethanation of CO<sub>2</sub>Chemical technologyTP1-1185ChemistryQD1-999ENCatalysts, Vol 11, Iss 1412, p 1412 (2021)
institution DOAJ
collection DOAJ
language EN
topic MIL-53–Al<sub>2</sub>O<sub>3</sub>
Ni/MIL-53 catalyst
Ni/MIL-53–Al<sub>2</sub>O<sub>3</sub> catalyst
methanation of CO<sub>2</sub>
Chemical technology
TP1-1185
Chemistry
QD1-999
spellingShingle MIL-53–Al<sub>2</sub>O<sub>3</sub>
Ni/MIL-53 catalyst
Ni/MIL-53–Al<sub>2</sub>O<sub>3</sub> catalyst
methanation of CO<sub>2</sub>
Chemical technology
TP1-1185
Chemistry
QD1-999
Oana Grad
Gabriela Blanita
Mihaela D. Lazar
Maria Mihet
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
description 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.
format article
author Oana Grad
Gabriela Blanita
Mihaela D. Lazar
Maria Mihet
author_facet Oana Grad
Gabriela Blanita
Mihaela D. Lazar
Maria Mihet
author_sort Oana Grad
title 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
title_short 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
title_full 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
title_fullStr 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
title_full_unstemmed 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
title_sort 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
publisher MDPI AG
publishDate 2021
url https://doaj.org/article/b4724aab9c6f45c2bf13fa393d63f258
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