title: A DFT Study of CO2Hydrogenation on Faujasite-Supported Ir4Clusters: on the Role of Water for Selectivity Control.
abstract: Reaction mechanisms for the catalytic hydrogenation of CO2by faujasite-supported Ir4clusters were studied by periodic DFT calculations. The reaction can proceed through two alternative paths. The thermodynamically favoured path results in the reduction of CO2to CO, whereas the other, kinetically preferred channel involves CO2hydrogenation to formic acid under water-free conditions. Both paths are promoted by catalytic amounts of water confined inside the zeolite micropores with a stronger promotion effect for the reduction path. Co-adsorbed water facilitates the cooperation between the zeolite Brønsted acid sites and Ir4cluster by opening low-energy reaction channels for CO2conversion.
authors.affiliation: Department of Chemical Engineering and Chemistry Eindhoven University of Technology Den Dolech 25612 MB Eindhoven The Netherlands; Division of Fuels Chemistry and Technology Faculty of Chemistry, Wrocław University of Technologyul. Gdańska 7/950-344 Wrocław Poland.
authors.forename: Bartłomiej M
authors.initials: BM
authors.lastname: Szyja
authors.affiliation: Division of Fuels Chemistry and Technology Faculty of Chemistry, Wrocław University of Technologyul. Gdańska 7/950-344WrocławPoland; Faculty of Mechanical and Power Engineering Wrocław University of TechnologyWybrzeże Wyspiańskiego 2750-370 Wrocław Poland.
authors.forename: Daniel
authors.initials: D
authors.lastname: Smykowski
authors.affiliation: Division of Fuels Chemistry and Technology Faculty of Chemistry, Wrocław University of Technology ul. Gdańska 7/9 50-344 Wrocław Poland.
authors.forename: Jerzy
authors.initials: J
authors.lastname: Szczygieł
authors.affiliation: Department of Chemical Engineering and Chemistry Eindhoven University of Technology Den Dolech 2 5612 MB Eindhoven The Netherlands.
authors.forename: Emiel J M
authors.initials: EJ
authors.lastname: Hensen
authors.affiliation: Department of Chemical Engineering and Chemistry Eindhoven University of Technology Den Dolech 25612 MB Eindhoven The Netherlands; Institute of Complex Molecular Systems Eindhoven University of Technology Den Dolech 25612 MB Eindhoven The Netherlands.
authors.forename: Evgeny A
authors.identifier: 0000-0001-9242-9901
authors.initials: EA
authors.lastname: Pidko
keywords: carbon storage; density functional calculations; hydrogenation; reaction mechanisms; zeolites