Methacrylic acid by carboxylation of propene with CO2 over POM catalysts - Reality or wishful thinking?

Rajagopalan P, Kühnle M, Polyakov M, Müller K, Arlt W, Kruse D, Brückner A, Bentrup U (2014)

Publication Status: Published

Publication Type: Journal article

Publication year: 2014

Journal

Catalysis Communications Elsevier

Publisher: Elsevier

Book Volume: 48

Pages Range: 19-23

DOI: 10.1016/j.catcom.2014.01.019

Abstract

Inspired by promising literature data on the production of methacrylic add (MAA) via heterogeneous selective gas-phase oxidation of propene by CO2, we performed a comprehensive study including in situ FTIR spectroscopy, catalytic tests as well as thermodynamic calculations using the same type of catalysts to reproduce these very surprising data and to further improve this process. Exemplarily, pure and supported Keggin type polyoxometalates (POM) Ni-3[PW12O40](2) and Ni-3[PMo12O40](2) were treated in different feeds containing CO2, propene/He, and propene/CO2/He. It was found that CO2 is only chemisorbed as surface carbonates but does not act as oxidizing agent. Instead, this role is played by lattice oxygen from the POM catalysts which, however, does not lead to the desired MAA target product but only to various unselective oxygenates including CO. Thermodynamic calculations clearly showed that reaction of COx with propene to MAA is not possible. Thus, this study clearly rebuts previous literature data. (C) 2014 Elsevier B.V. All rights reserved.

Authors with CRIS profile

Karsten Müller Lehrstuhl für Thermische Verfahrenstechnik Wolfgang Arlt Lehrstuhl für Thermische Verfahrenstechnik

Involved external institutions

Leibniz-Institut für Katalyse (LIKAT) / Leibniz Institute for Catalysis DE Germany (DE) Evonik Degussa GmbH DE Germany (DE)

How to cite

APA:

Rajagopalan, P., Kühnle, M., Polyakov, M., Müller, K., Arlt, W., Kruse, D.,... Bentrup, U. (2014). Methacrylic acid by carboxylation of propene with CO2 over POM catalysts - Reality or wishful thinking? Catalysis Communications, 48, 19-23. https://doi.org/10.1016/j.catcom.2014.01.019

MLA:

Rajagopalan, Prasanna, et al. "Methacrylic acid by carboxylation of propene with CO2 over POM catalysts - Reality or wishful thinking?" Catalysis Communications 48 (2014): 19-23.

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