Selective Methanol Carbonylation to Acetic Acid on Heterogeneous Atomically Dispersed ReO4 /SiO2 Catalysts

Journal of the American Chemical Society
Ji QiPhillip Christopher

Abstract

Methanol carbonylation to acetic acid (AA) is a large-scale commodity chemical production process that requires homogeneous liquid-phase organometallic catalysts with corrosive halide-based cocatalysts to achieve high selectivity and activity. Here, we demonstrate a heterogeneous catalyst based on atomically dispersed rhenium (ReO4) active sites on an inert support (SiO2) for the halide-free, gas phase carbonylation of methanol to AA. Atomically dispersed ReO4 species and nanometer sized ReO x clusters were deposited on a high surface area (700 m2/g) inert SiO2 using triethanolamine as a dispersion promoter and characterized using aberration corrected scanning transmission electron microscopy (AC-STEM), UV-vis spectroscopy, and X-ray absorption spectroscopy (XAS). Reactivity measurements at atmospheric pressure with 30 mbar of methanol and CO (1:1 molar ratio) showed that bulk Re2O7 and ReO x clusters on SiO2 (formed at >10 wt %) were selective for dimethyl ether formation, while atomically dispersed ReO4 on SiO2 (formed at <10 wt %) exhibited stable (for 60 h) > 93% selectivity to AA with single pass conversion >60%. Kinetic analysis, in situ FTIR, and in situ XAS measurements suggest that the AA formation mechanism involves...Continue Reading

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Dec 10, 2019·Journal of the American Chemical Society·Joaquin ResascoPhillip Christopher

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Citations

Sep 15, 2020·Journal of the American Chemical Society·Shuchen ZhangGabor A Somorjai
Oct 29, 2020·Chemical Reviews·Rui LangTao Zhang

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