Journal of Siberian Federal University. Chemistry / Methane Catalytic Peroxide Oxidation Over Fe-Containing Zeolite

Full text (.pdf)
Issue
Journal of Siberian Federal University. Chemistry. 2016 9 (4)
Authors
Boltenkov, Vadim V.; Taran, Oxana P.; Parkhomchuk, Ekaterina V.; Yashnik, Svetlana A.; Sashkina, Kseniya A.; Ayusheev, Artemiy B.; Babushkin, Dmitrii E.; Parmon, Valentin N.
Contact information
Boltenkov, Vadim V.: Boreskov Institute of Catalysis SB RAS 5 Akad. Lavrentiev, Novosibirsk, 630090, Russia; ; Taran, Oxana P.:Boreskov Institute of Catalysis SB RAS 5 Lavrentieva, Novosibirsk, 630090, Russia; Novosibirsk State Technical University; Novosibirsk State Technical University 20 Karl Marx, Novosibirsk, 630092, Russia; Parkhomchuk, Ekaterina V.: Boreskov Institute of Catalysis SB RAS 5 Akad. Lavrentiev, Novosibirsk, 630090, Russia; Novosibirsk State University 2 Pirogova Str., Novosibirsk, 630090, Russia; Yashnik, Svetlana A.: Boreskov Institute of Catalysis SB RAS 5 Akad. Lavrentiev, Novosibirsk, 630090, Russia; Sashkina, Kseniya A.: Boreskov Institute of Catalysis SB RAS 5 Akad. Lavrentiev, Novosibirsk, 630090, Russia; Ayusheev, Artemiy B.: Boreskov Institute of Catalysis SB RAS 5 Lavrentieva, Novosibirsk, 630090, Russia; ; Babushkin, Dmitrii E.: Boreskov Institute of Catalysis SB RAS 5 Akad. Lavrentiev, Novosibirsk, 630090, Russia; Parmon, Valentin N.:Boreskov Institute of Catalysis SB RAS 5 Akad. Lavrentiev, Novosibirsk, 630090, Russia; Novosibirsk State University 2 Pirogova Str., Novosibirsk, 630090, Russia
Keywords
Fe-ZSM-5; methane; formic acid; methanol; Fe-ZSM-5; Fe-silicalite; peroxide oxidation
Abstract

The selectivity of Fe-MFI catalysts to partial peroxide oxidation of methane to methanol and formic acid was studied depending on their topology (Nanocrystals, Microcrystals, and bulk Commercial) and activation with oxalic acid. The catalysts were characterized by XRD, ICP-OES, SEM, UV-vis DR, NH3-TPD, N2 adsorption. TOF of methane oxidation increased in the series: Nanocrystals < Microcrystals << Commercial. The selectivity to methanol depended mainly on the crystallite size and increased in the same series. The increase in TOF and selectivity to formic acid, as well as a sharp decrease in the selectivity to CO2 over all the activated catalysts were accounted for by an increase in the total acidity of the catalysts and the number of oligomeric Fe oxo-clusters. Different pathways to the formation of methanol/CO2 (via free radical mechanism) and formic acid (via heterogeneous route) over Fe-MFI catalysts were suggested

Pages
394-413
Paper at repository of SibFU
https://elib.sfu-kras.ru/handle/2311/32099