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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2021
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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) |
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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 |
work_keys_str_mv |
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_version_ |
1718412735419514880 |