Ceria Nanostructured Catalysts for Conversion of Methanol and Carbon Dioxide to Dimethyl Carbonate

Author

Jawad Al-Darwish
Matthew Senter
Shane Lawson
Fateme Rezaei, Missouri University of Science and TechnologyFollow
Ali A. Rownaghi, Missouri University of Science and TechnologyFollow

Abstract

In this study, ceria (CeO₂) with three different shapes (nanooctahedra, nanocubes, nanorods) was synthesized via hydrothermal method and evaluated for carbonylation reaction. Off these three nanostructures, the nanorod ceria was doped with CaO, NiO, CuO, and CoO by wet impregnation method. The obtained catalysts were characterized by X-ray diffraction (XRD), NH₃/CO₂-TPD, X-ray fluorescence (XRF), Fourier Transform Infrared Spectroscopy (FTIR), and N₂ physisorption to determine the crystal size and phases, acid-base properties, metal loading, and surface properties. The materials were used as catalyst for activation of CO₂ and methanol carbonylation reaction to dimethyl carbonate (DMC) at 140 °C and 30 bar for a reaction duration of 3 h. Our results indicated that the shape of the nanostructured ceria influences the DMC yield with the CeO₂ nanorod catalyst producing the highest DMC yield (1.6 mmol) followed by nanooctahedra (1.5 mmol) and nanocubes (1.0 mmol). Moreover, the catalytic tests showed 100% DMC selectivity and the catalytic activities showed a decreasing trend in the following order: CeO₂ > CoO/CeO₂ > NiO/CeO₂ > CaO/CeO₂ > CuO/CeO₂. The materials characterization and evaluation results suggested that CeO₂ nanorod (111) interface enhanced the surface basicity and activity of CO₂ hydrogenation to methanol while the CeO₂ octahedral sites improved the stability of catalyst. The reusability of the CeO₂ was tested by conducting four consecutive cycles and it was noted that the catalytic activity of CoO/CeO₂ remained relatively stable with small changes after each run.

Recommended Citation

J. Al-Darwish et al., "Ceria Nanostructured Catalysts for Conversion of Methanol and Carbon Dioxide to Dimethyl Carbonate," Catalysis Today, vol. 350, pp. 120 - 126, Elsevier B.V., Jun 2020.

The definitive version is available at https://doi.org/10.1016/j.cattod.2019.06.013

Department(s)

Chemical and Biochemical Engineering

Keywords and Phrases

Bimetallic catalysts; Ceria nanostructures; CO2utilization; Dimethyl carbonate synthesis; Methanol carbonylation

International Standard Serial Number (ISSN)

0920-5861

Document Type

Article - Journal

Document Version

Citation

File Type

text

Language(s)

English

Rights

© 2019 Elsevier B.V., All rights reserved.

Publication Date

15 Jun 2020