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Temperature-programmed Deoxygenation of Acetic Acid on Molybdenum Carbide Catalysts
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Selective Methanol Carbonylation to Acetic Acid on Heterogeneous Atomically Dispersed ReO4/SiO2 Catalysts
Ji Qi1, Jordan Finzel1, Hossein Robatjazi1
1Department of Chemical Engineering, University of California, Santa Barbara, Santa Barbara, California 93117, United States.
Journal of the American Chemical Society
|July 22, 2020
Summary
This study introduces a novel heterogeneous catalyst using atomically dispersed rhenium on silica for methanol carbonylation to acetic acid, achieving high selectivity and activity without corrosive halides.
Area of Science:
- Catalysis
- Materials Science
- Chemical Engineering
Background:
- Methanol carbonylation to acetic acid typically uses homogeneous catalysts with corrosive halide promoters.
- Developing efficient heterogeneous catalysts for this process is crucial for industrial applications.
Purpose of the Study:
- To develop a halide-free, heterogeneous catalyst for methanol carbonylation to acetic acid.
- To investigate the performance and mechanism of atomically dispersed rhenium oxide species on silica supports.
Main Methods:
- Synthesis of atomically dispersed ReO4 on SiO2 using triethanolamine.
- Characterization using AC-STEM, UV-vis spectroscopy, and XAS.
- Reactivity measurements, kinetic analysis, in situ FTIR, and in situ XAS.
Main Results:
- Atomically dispersed ReO4 on SiO2 demonstrated >93% selectivity to acetic acid with >60% conversion.
- The catalyst showed stable performance for 60 hours in gas-phase methanol carbonylation.
- Addition of Rh promoter further enhanced selectivity to >96%.
Conclusions:
- Atomically dispersed ReO4 on inert SiO2 represents a promising halide-free heterogeneous catalyst for acetic acid production.
- The proposed mechanism involves methanol activation and CO insertion.
- This work opens avenues for new heterogeneous catalysts in alcohol carbonylation.
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