Product selectivity and mass transport in levulinic acid transfer hydrogenation by monolithic MIL-100, MIL-88B and ZIF-8Pd MOFs
Copyright © 2023 McIntyre, Saenz-Cavazos, Hunter-Sellars, Williams..
The diffusion processes between adsorbent and adsorbate naturally play a significant role in the efficiency and selectivity of the heterogenous catalytic process. This paper considers the importance of diffusion processes in the transfer hydrogenation reaction of levulinic acid to γ-valerolactone by MIL-88B, MIL-100, and ZIF8Pd monolithic catalysts. Over a period of five catalytic cycles, it was shown that the Fe-based catalysts can achieve similar conversions to the ZIF-8 supported Pd, with the only current limitation being the lower aqueous stability of these MOFs. Diffusion constants were calculated using the ZLC method, with micropore diffusion limitation found for ZIF-8 and MIL-100 monolithic frameworks at 2.7 x 10-8 and 4.6 x 10-8 cm2 s-1 respectively. This diffusion limitation was also confirmed by IR spectroscopy with an increasing concentration of C-H bands on the MOF substrate post-reaction. Mass transfer coefficients, also calculated by ZLC, revealed increased mass transport for the hydrophobic ZIF-8 framework, which perhaps aids in the γ-valerolactone selectivity over side products that are produced in the absence of catalytic material, as seen for MIL-88B and MIL-100 after multiple uses.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2022 |
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| Erschienen: |
2022 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:10 |
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| Enthalten in: |
Frontiers in chemistry - 10(2022) vom: 20., Seite 1087939 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
McIntyre, Sean R [VerfasserIn] |
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| Links: |
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| Themen: |
Biomass conversion |
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| Anmerkungen: |
Date Revised 02.02.2023 published: Electronic-eCollection Citation Status PubMed-not-MEDLINE |
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| doi: |
10.3389/fchem.2022.1087939 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM352234032 |
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| 100 | 1 | |a McIntyre, Sean R |e verfasserin |4 aut | |
| 245 | 1 | 8 | |a Product selectivity and mass transport in levulinic acid transfer hydrogenation by monolithic MIL-100, MIL-88B and ZIF-8Pd MOFs |
| 264 | 1 | |c 2022 | |
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| 500 | |a Date Revised 02.02.2023 | ||
| 500 | |a published: Electronic-eCollection | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a Copyright © 2023 McIntyre, Saenz-Cavazos, Hunter-Sellars, Williams. | ||
| 520 | |a The diffusion processes between adsorbent and adsorbate naturally play a significant role in the efficiency and selectivity of the heterogenous catalytic process. This paper considers the importance of diffusion processes in the transfer hydrogenation reaction of levulinic acid to γ-valerolactone by MIL-88B, MIL-100, and ZIF8Pd monolithic catalysts. Over a period of five catalytic cycles, it was shown that the Fe-based catalysts can achieve similar conversions to the ZIF-8 supported Pd, with the only current limitation being the lower aqueous stability of these MOFs. Diffusion constants were calculated using the ZLC method, with micropore diffusion limitation found for ZIF-8 and MIL-100 monolithic frameworks at 2.7 x 10-8 and 4.6 x 10-8 cm2 s-1 respectively. This diffusion limitation was also confirmed by IR spectroscopy with an increasing concentration of C-H bands on the MOF substrate post-reaction. Mass transfer coefficients, also calculated by ZLC, revealed increased mass transport for the hydrophobic ZIF-8 framework, which perhaps aids in the γ-valerolactone selectivity over side products that are produced in the absence of catalytic material, as seen for MIL-88B and MIL-100 after multiple uses | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a MOF | |
| 650 | 4 | |a biomass conversion | |
| 650 | 4 | |a diffusion constant | |
| 650 | 4 | |a hydrogenation | |
| 650 | 4 | |a mass transfer | |
| 650 | 4 | |a stability | |
| 650 | 4 | |a zero-length column | |
| 700 | 1 | |a Saenz-Cavazos, Paola A |e verfasserin |4 aut | |
| 700 | 1 | |a Hunter-Sellars, Elwin |e verfasserin |4 aut | |
| 700 | 1 | |a Williams, Daryl R |e verfasserin |4 aut | |
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