Issue 18, 2024

Superacidity in Zr(iv)/Ce(iii) MOF-808: unlocking biodiesel production from microalgae lipids at reduced temperatures

Abstract

To manage production costs and lower the conversion temperature of microalgal lipids, this study engineered superacid sites in MOF-808, facilitating lipid transformation at markedly reduced temperatures. Through simple substitution and activation steps, secondary building units formed by Zr(IV) and Ce(III) were assembled with benzene-1,3,5-tricarboxylate ligands, resulting in a unique superacid structure. This superacid structure has a Hammett acidity value of less than −14.5 and a deprotonation energy of 1016.25 kJ mol−1, both lower than those of sulfuric acid. Density functional theory and solid-state NMR analyses confirmed the superacidity arises from a weakly constrained superacid proton within a bridging structure, formed by two methanol molecules attracted to adjacent Ce and Zr atoms. Variable temperature infrared spectroscopy demonstrated the low-temperature activation of methanol, with the optimal reaction temperature reduced from 200 °C to 150 °C and pressure reduced by 2952 kPa. Unlike traditional solid superacids, this methanol-based superacid configuration prevents the loss of superacid sites, maintaining over 97% efficiency after five cycles.

Graphical abstract: Superacidity in Zr(iv)/Ce(iii) MOF-808: unlocking biodiesel production from microalgae lipids at reduced temperatures

Supplementary files

Article information

Article type
Paper
Submitted
27 Apr 2024
Accepted
22 Jul 2024
First published
09 Aug 2024

Catal. Sci. Technol., 2024,14, 5278-5290

Superacidity in Zr(IV)/Ce(III) MOF-808: unlocking biodiesel production from microalgae lipids at reduced temperatures

L. Qian, J. Cheng, K. Xin, Y. Mao, J. Tu and W. Yang, Catal. Sci. Technol., 2024, 14, 5278 DOI: 10.1039/D4CY00545G

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