Product selectivity and mass transport in levulinic acid transfer hydrogenation by monolithic MIL-100, MIL-88B and ZIF-8@Pd MOFs

Front Chem. 2023 Jan 12;10:1087939. doi: 10.3389/fchem.2022.1087939. eCollection 2022.


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 ZIF8@Pd 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.

PMID:36712992 | PMC:PMC9879703 | DOI:10.3389/fchem.2022.1087939


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