Hello everyone! My name is Domenico Aceto, an overenthusiastic scientist who always strives to unravel what makes nature’s cogs tick. I originally come from Bari, a city in southern Italy, where I graduated in Chemistry for both my Bachelor and Master’s degree. I studied the applications of plasmas on materials, ranging from the engineering to the biomedical field, and in the process remained fascinated with the endless potential that plasmas offer to human life. The pursuit of knowledge always pushed me forward, so at the end of my studies I knew I wanted to take on a PhD. This was when I learnt about the PIONEER program, which looked to me like an outstanding way to couple my desire to continue working on plasmas with the possibility of concretely helping out humanity in the current climate change crisis offering solutions to deal with CO2, one of the most dangerous greenhouse gas. Shifting how CO2 is perceived, from dangerous waste to useful resource, is in fact a key challenge for the future. This may seems way too ambitious to you, but just wait a couple of decades until all PIONEER ESRs will be awarded with the Nobel prize!
Nowadays I am a PhD student at Instituto Superior Técnico (IST-CATHPRO) in Lisbon, Portugal, as a part of the aforementioned MSCA PIONEER program. My research focuses on the design of innovative catalysts for the CO2 methanation reaction, with the goal to couple them with plasma to unlock and discover new properties and ways to enhance the reaction that cannot be achieved under conventional thermal catalysis. Moreover, I will be taking a closer look at those systems (catalysts under plasma) utilizing OPERANDO FT-IR spectroscopy at the CNRs-LCS laboratories in Caen, France. These measurements will be of great help to understand the reaction mechanism, which is not fully understood yet. I hope that my work, in association with the one of all the participants in the PIONEER program, will help bring a brighter and better future to us all, so wish all of us good luck!
| Overview |  |
| ESR: | 5 |
| Title: | Ru-based catalysts for plasma-assisted CO2 methanation |
| Home Institution: | Instituto Superior Técnico Lisboa (IST-CATHPRO ) |
| 1st Supervisor: | Carlos Henriques |
| Host Institution: | Laboratoire Catalyse & Spectrochimie (CNRS-LCS) |
| 2nd Supervisor: | Federico Azzolina-Jury |
| Industrial Partner: | Green Syn Fuel |
| Industrial Contact: | José João Campos Rodrigues |
| Defence: | May 17 2024 |
Abstract
In this work, novel catalysts to carry out the plasma-assisted CO2 methanation reaction (Sabatier reaction) were designed and tested. In fact, CO2 is a very interesting reactant in hydrogenation reactions because of its production by human industrial activity and the necessity to remove it from the atmosphere, where it acts as a greenhouse gas, while the produced CH4 has many advantages as well, including already having an existing distribution network. The traditionally thermally activated reaction could be further enhanced by the utilisation of Dielectric Barrier Discharge (DBD) plasma-induced catalysis in the presence of a catalyst material. Thus, different classes of Ru-based catalysts, supported over microporous zeolites (USY, BEA, MOR and ZSM-5) and mesoporous silicas (SBA-15 and MCM-41), were designed, synthesized and tested in both thermal and plasma-assisted catalysis conditions. Indeed, the catalyst prepared using 3% in weight of Ru dispersed by incipient wetness impregnation over USY zeolite having a Si/Al ratio of 38 and Cs as a compensating cation was found to be the best one in both environments, pointing out to many properties of the support material (hydrophobicity, basicity and porosity) to be critical in defining a well-performing catalyst. Moreover, a heavy focus on the reaction mechanism was put on this study, by means of in-situ operando FTIR, which was possible under plasma-catalysis conditions thanks to the design of a novel DBD Transmission-FTIR cell. The proposed mechanism, under plasma-catalysis conditions involves the dissociation of CO2 in the plasma and its adsorption on the surface of the catalysts as carbonates or carbonyls species, that are then progressively reduced to formates and then to methane. This mechanism is quite similar to the one observed under thermal catalysis conditions, likely due to the mild conditions (temperature) created by the DBD plasma, that nonetheless unlocks adsorption and reaction pathways happening on the supported material alone, not observed before.
Links with other ESRs
- ESR 1: Comparison with results for correlation between surface electric field and surface reactivity as well as important data for the design of catalyst
Secondments
- CNRS-LCS: Obtaining in-situ IR measurements with the OPERANDO setup from CNRS-LCS for the catalytic materials developed at IST-CATHPRO
- Green Syn Fuel: Realistic design of industrial reactors