Aqueous phase conversion of CO2 into acetic acid over thermally transformed MIL-88B catalyst

Waqar Ahmad, Paramita Koley, Swarit Dwivedi, Rajan Lakshman, Yun Kyung Shin, Adri C. T. Duin, Abhijit Shrotri and Akshat Tanksale ()
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Waqar Ahmad: Monash University
Paramita Koley: Monash University
Swarit Dwivedi: Monash University
Rajan Lakshman: Monash University
Yun Kyung Shin: The Pennsylvania State University
Adri C. T. Duin: The Pennsylvania State University
Abhijit Shrotri: Hokkaido University
Akshat Tanksale: Monash University

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Sustainable production of acetic acid is a high priority due to its high global manufacturing capacity and numerous applications. Currently, it is predominantly synthesized via carbonylation of methanol, in which both the reactants are fossil-derived. Carbon dioxide transformation into acetic acid is highly desirable to achieve net zero carbon emissions, but significant challenges remain to achieve this efficiently. Herein, we report a heterogeneous catalyst, thermally transformed MIL-88B with Fe0 and Fe3O4 dual active sites, for highly selective acetic acid formation via methanol hydrocarboxylation. ReaxFF molecular simulation, and X-ray characterisation results show a thermally transformed MIL-88B catalyst consisting of highly dispersed Fe0/Fe(II)-oxide nanoparticles in a carbonaceous matrix. This efficient catalyst showed a high acetic acid yield (590.1 mmol/gcat.L) with 81.7% selectivity at 150 °C in the aqueous phase using LiI as a co-catalyst. Here we present a plausible reaction pathway for acetic acid formation reaction via a formic acid intermediate. No significant difference in acetic acid yield and selectivity were noticed during the catalyst recycling study up to five cycles. This work is scalable and industrially relevant for carbon dioxide utilisation to reduce carbon emissions, especially when green methanol and green hydrogen are readily available in future.

Date: 2023
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DOI: 10.1038/s41467-023-38506-5

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