Periodic Reporting for period 2 - MECHANISM (The effect of water on the Fischer-Tropsch reaction mechanism and kinetics over bimetallic Co-based catalysts: Theoretical and experimental studies)
Période du rapport: 2019-04-03 au 2020-04-02
This project has six objectives: (1) the training and career development of the researcher; (2) the synthesis of bimetallic Co-based catalysts of uniform composition and a range of mean cluster diameter; (3) the physicochemical characterization of bimetallic Co-based catalytic materials, using TEM, PXRD, BET and TPD; (4) the understanding of the influence of water on the catalytic behaviour of these catalytic materials; (5) the elucidation of mechanistic details using DFT calculations, SSITKA-DRIFTS and -MS technique and transient experiment in order to study the effect of water, support structure and cluster size on the nature and reactivity of reaction intermediates; (6) the dissemination of results and public engagements.
The MECHANISM project results were presented to society by participation in the European Researcher’s Night, thought a video, an article in local magazines, a website (http://www.mechanism.ucy.ac.cy) and a lecture to undergraduate students (Marie Curie Ambassador). In addition, the results were presented to the scientific community thought six (6) scientific publications in peer-reviewed international scientific journals of high impact factor, one (1) presentation in international conference and five (5) presentations in the department.
H2O does not significantly affect the concentration and chemical structure on active and inactive species (SSITKA-MS, -DRIFTS, TIH/TPH). The surface coverage of inactive species are constant with Co nanoparticle size and increased with increasing time on stream (TOS). The surface coverage of active CO-s and CHx-s increased with Co nanoparticle size. On the contrary, the surface coverage of active CO-s stayed practically constant and that of CHx-s decreased with increasing TOS. The main reason of catalyst deactivation was the accumulation of inactive -CxHy with TOS that may affect the binding strength of co-adsorb active intermediates or may occupy sites where active species can formed. The D-KIE estimated by a novel 13CO/D2-SSITKA experiment and gave an inverse D-KIE for CO consumption and CH4 formation, independent of dCO.
This project is important from an economic point of view since the price of crude oil is rising frequently (production of synthetic fuels) and the development of more active and selective FTS catalysts would offer an alternative given the environmental advantages of fuels derived from FTS. The results of this project are considered very important and strongly linked to the European energy needs.