Computational Mechanism of Methyl Levulinate Conversion to γ-Valerolactone on UiO-66 Metal Organic Frameworks

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2022_acssuschemeng_ortuno_computational.pdf (1.98 MB)
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URI: http://hdl.handle.net/10347/29211
ISSN: 2168-0485
DOI: 10.1021/acssuschemeng.1c08021

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2022

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ACS Publications
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Abstract

Metal–organic frameworks (MOFs) are gaining importance in the field of biomass conversion and valorization due to their porosity, well-defined active sites, and broad tunability. But for a proper catalyst design, we first need detailed insight of the system at the atomic level. Herein, we present the reaction mechanism of methyl levulinate to γ-valerolactone on Zr-based UiO-66 by means of periodic density functional theory (DFT). We demonstrate the role of Zr-based nodes in the catalytic transfer hydrogenation (CTH) and cyclization steps. From there, we perform a computational screening to reveal key catalyst modifications to improve the process, such as node doping and linker exchange

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Density functional theory (DFT)| Metal organic framework (MOF)| Catalyst design| Biomass valorization| Catalytic transfer hydrogenation (CTH)

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ACS Sustainable Chem. Eng. 2022, 10, 11, 3567–3573

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This work has received financial support from the Beatriu de Pinós postdoctoral program of the Government of Catalonia’s Secretariat for Universities and Research (2017-BP-00039), MINECO (under project PID2020-119116RA-I00), Xunta Distinguished Researcher program (ED431H 2020/21), the Xunta de Galicia (Centro singular de investigación de Galicia accreditation 2019-2022, ED431G 2019/03), and the European Union (European Regional Development Fund - ERDF). R.L. gratefully acknowledges funding from MINECO under project PID2019-109953GB-I00

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© 2022 The Authors. Published by American Chemical Society. This work is under a CC Attribution 4.0 International license (CC BY 4.0) (http://creativecommons.org/licenses/by/4.0/)
Atribución 4.0 Internacional

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Centro de Investigación en Química Biolóxica e Materiais Moleculares (CiQUS)
Química Orgánica