Ortuño Maqueda, Manuel ÁngelRellán Piñeiro, MarcosLuque, Rafael2022-09-062022-09-062022ACS Sustainable Chem. Eng. 2022, 10, 11, 3567–35732168-0485http://hdl.handle.net/10347/29211Metal–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 exchangeeng© 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 Internacionalhttp://creativecommons.org/licenses/by/4.0/Density functional theory (DFT)Metal organic framework (MOF)Catalyst designBiomass valorizationCatalytic transfer hydrogenation (CTH)journal article10.1021/acssuschemeng.1c08021open access