Lukas D. Ernst, Christian Njel, Wijnand Marquart, Shaine Raseale, Michael Claeys, Nico Fischer, Ingo Krossing
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引用次数: 0
Abstract
Oxidative fluorination is reported to increase methanol (MeOH) productivity of binary copper–zinc oxide (CZ) catalyst systems yet is incompatible with all the hitherto tested ternary support materials. Here, we show that the oxidative fluorination with F2 gas of CZ MeOH catalysts including iron oxide as a support material improves catalytic performances. A systematic variation of the compositions of the investigated ternary CZFe (copper, zinc, and iron) catalyst system led to a total of 13 different systems. The subsequent oxidative fluorination of all systems with a low F2 pressure of 200 mbar showed significant improvement in the MeOH productivity and selectivity for almost all systems tested. High-iron systems benefited most from oxidative fluorination. In addition, selected systems were exposed to higher F2 amounts and were studied. Further measurements showed that the crystallinity, surface area, and high-temperature carbonate content of the CZFe systems are very well tunable. Kinetic investigations indicated that fluorination leads to an increase in the number of active sites for the MeOH synthesis and at the same time increases the apparent activation energy for the RWGS reaction. In addition, oxidative fluorination at total F2 pressures of and higher than 1250 mbar shuts down the iron-induced parasitic Fischer–Tropsch-type hydrogenation to hydrocarbons and results in the highest MeOH production rates.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.