Nanoconfinement for production of platform molecules from carbon oxides ; Nanoconfinement pour la synthèse de molécules plateforme à partir des oxydes de carbone

Energy and environmental impacts drove the industrial processes. A sustainable route to produce fuels starts using biomass as raw material. Fischer-Tropsch synthesis is a promising alternative way for conversion of renewable feedstocks to chemicals and fuels. Even FT synthesis is considered a well-established technology, there are chemistry fundamentals to be better and deeply understood. Besides, the FT process depends strongly on the catalyst performance. The utilization and transformation of CO2 into value-added chemicals have been of global interest, from both theoretical and practical viewpoints. One example of CO2 conversion to a useful liquid hydrocarbon is hydrogenation of CO2 to formic acid (HCOOH). The state-of-the-art hydrogenation of CO2 to formic acid is produced over homogeneous catalysts. However, there are a few works showing that highly dispersed supported metal catalysts are able to carry out this reaction. The high activity of these catalysts could be assigned to their ability to stabilize the active metal in a state of single-metal atoms or heterogenized metal complexes, which may demonstrate a higher activity than metal atoms on the surface of metal nanoparticles.In this work we have considered two different confined spaces of carbon-based materials, CNTs and COFs, and evaluated the nanoconfinement of iron, copper and ruthenium active species for CO and CO2 hydrogenation reactions to produce value-added chemicals and platform molecules.In the iron catalysts for FT synthesis supported by carbon nanotubes, the active phase was nanoconfined inside the channels or localized on the outer surface. In most of previous work, the distribution of metal nanoparticles inside or outside carbon nanotubes is considered to be immobile during the catalyst activation or catalytic reaction. In this work, we uncovered remarkable mobility of both iron and copper species in the bimetallic catalysts between inner carbon nanotube channels and outer surface, which occurs in carbon monoxide and syngas, while almost ...