The 2020 plasma catalysis roadmap

International audienc

Meta-analysis of CO2 conversion, energy efficiency, and other performance data of plasma-catalysis reactors with the open access PIONEER database

This paper brings the comparison of performances of CO2 conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field, organised in an open access online database. This tool is open to all users to carry out their own analyses, but also to contributors who wish to add their data to the database in order to improve the relevance of the comparisons made, and ultimately to improve the efficiency of CO2 conversion by plasma-catalysis. The creation of this database and database user interface is motivated by the fact that plasma-catalysis is a fast-growing field for all CO2 conversion processes, be it methanation, dry reforming of methane, methanolisation, or others. As a result of this rapid increase, there is a need for a set of standard procedures to rigorously compare performances of different systems. However, this is currently not possible because the fundamental mechanisms of plasma-catalysis are still too poorly understood to define these standard procedures. Fortunately however, the accumulated data within the CO2 plasma-catalysis community has become large enough to warrant so-called “big data” studies more familiar in the fields of medicine and the social sciences. To enable comparisons between multiple data sets and make future research more effective, this work proposes the first database on CO2 conversion performances by plasma-catalysis open to the whole community. This database has been initiated in the framework of a H2020 European project and is called the “PIONEER DataBase”. The database gathers a large amount of CO2 conversion performance data such as conversion rate, energy efficiency, and selectivity for numerous plasma sources coupled with or without a catalyst. Each data set is associated with metadata describing the gas mixture, the plasma source, the nature of the catalyst, and the form of coupling with the plasma. Beyond the database itself, a data extraction tool with direct visualisation features or advanced filtering functionalities has been developed and is available online to the public. The simple and fast visualisation of the state of the art puts new results into context, identifies literal gaps in data, and consequently points towards promising research routes. More advanced data extraction illustrates the impact that the database can have in the understanding of plasma-catalyst coupling. Lessons learned from the review of a large amount of literature during the setup of the database lead to best practice advice to increase comparability between future CO2 plasma-catalytic studies. Finally, the community is strongly encouraged to contribute to the database not only to increase the visibility of their data but also the relevance of the comparisons allowed by this tool

Novel boehmite transformation into γ-alumina and preparation of efficient nickel base alumina porous extrudates for plasma-assisted CO2 methanation

International audienc

Synthesis and characterization of zeolites modified with transition metals : Dielectric and magnetic properties measurements and their application to the synthesis of chemical compounds under microwave irradiation

Cette étude est centrée sur la synthèse et la préparation de zéolithes modifiées par des métaux de transition avec leurs applications en catalyse sous irradiation microondes. Des travaux précédents ont montré l’intérêt de modifier des zéolithes avec des métaux de transition pour leur application sur des réactions d’oxydation et d’utiliser les microondes afin d’augmenter les vitesses de réaction. Dans cette thèse, nous avons étudié deux types de structure zéolithique (MEL et FAU) dopés par des métaux de transition (Co, Mn, Fe, Zn, Ni, Cr) à différentes concentrations. Une étude classique de caractérisation a permis d’augmenter la connaissance sur la préparation de zéolithes modifiées et de comprendre leur influence sur l’activité catalytique. La réaction d’oxydation partielle du styrène pour la production du benzaldéhyde a été choisie comme réaction modèle. La zéolithe Co-ZSM-11 a présenté la meilleure activité catalytique dans cette étude ainsi que par rapport à d’autres catalyseurs présentés dans la littérature.Les réactions d’oxydation du styrène ont été étudiées sous irradiation microondes et sous chauffage conventionnel. Aucune différence sur l’activité des zéolithes dopées n’a été observée pour les deux types de chauffage. Les faibles valeurs de permittivités et perméabilités des zéolithes dopées par des métaux de transition rendent difficile l’intensification du procédé d’obtention de benzaldéhyde à partir de l’oxydation du styrène sous microondes. Les paramètres de la réaction modèle ont été optimisés et une étude cinétique a été menée avec la zéolithe Co-ZSM-11. Enfin, le chauffage par hystérésis diélectrique a été utilisé dans la synthèse de zéolithes ZSM-11. Le temps de synthèse a été considérablement réduit (80%) par rapport au temps nécessaire sous chauffage conventionnel.This study focuses on the synthesis and preparation of modified zeolites with transition metals and theirs applications in catalysis under microwave irradiation. Previous works have shown interest in modifying zeolites with transition metals for their application to oxidation reactions and in using microwave irradiation in order to increase the reaction rates. In this thesis, we studied two types of zeolite structure (MEL and FAU) doped with transitionmetals (Co, Mn, Fe, Zn, Ni, Cr) at different concentrations. A classic characterization study has increased the knowledge on the preparation of modified zeolites and the understanding of their influence on thecatalytic activity. The styrene partial oxidation reaction for benzaldehyde production was chosen as amodel reaction. Co-ZSM-11 zeolite presented the best catalytic activity in this study and also compared to other catalysts found in the literature. The styrene oxidation reactions were studied under microwave irradiation and under conventional heating. No difference in the activity of doped zeolites was observed for both types of heating. The low values of permittivity and permeability of zeolites doped with transition metals make difficult the intensification of the benzaldehyde production process from styrene oxidation under microwave. The parameters of the model reaction have been optimized and a reaction kinetic study was carried out by using the Co-ZSM-11 zeolite. Finally, the hysteresis dielectric heating was used in the synthesis of ZSM-11. The synthesis time was significantly reduced (80%) under microwave irradiation compared to conventional heating

Influence of Microwave-Assisted Synthesis Parameters on ZSM-11 Zeolite Production Without Seeding

International audienc

Mechanism of Low Pressure Plasma-Assisted CO2 Hydrogenation Over Ni-USY by Microsecond Time-resolved FTIR Spectroscopy

International audienc

Préparation et caractérisation de zéolithes dopées par des métaux de transition (Mesure de propriétés diélectriques et magnétiques et leur application à la synthèse de composés chimiques sous irradiation microondes)

Cette étude est centrée sur la synthèse et la préparation de zéolithes modifiées par des métaux de transition avec leurs applications en catalyse sous irradiation microondes. Des travaux précédents ont montré l intérêt de modifier des zéolithes avec des métaux de transition pour leur application sur des réactions d oxydation et d utiliser les microondes afin d augmenter les vitesses de réaction. Dans cette thèse, nous avons étudié deux types de structure zéolithique (MEL et FAU) dopés par des métaux de transition (Co, Mn, Fe, Zn, Ni, Cr) à différentes concentrations. Une étude classique de caractérisation a permis d augmenter la connaissance sur la préparation de zéolithes modifiées et de comprendre leur influence sur l activité catalytique. La réaction d oxydation partielle du styrène pour la production du benzaldéhyde a été choisie comme réaction modèle. La zéolithe Co-ZSM-11 a présenté la meilleure activité catalytique dans cette étude ainsi que par rapport à d autres catalyseurs présentés dans la littérature.Les réactions d oxydation du styrène ont été étudiées sous irradiation microondes et sous chauffage conventionnel. Aucune différence sur l activité des zéolithes dopées n a été observée pour les deux types de chauffage. Les faibles valeurs de permittivités et perméabilités des zéolithes dopées par des métaux de transition rendent difficile l intensification du procédé d obtention de benzaldéhyde à partir de l oxydation du styrène sous microondes. Les paramètres de la réaction modèle ont été optimisés et une étude cinétique a été menée avec la zéolithe Co-ZSM-11. Enfin, le chauffage par hystérésis diélectrique a été utilisé dans la synthèse de zéolithes ZSM-11. Le temps de synthèse a été considérablement réduit (80%) par rapport au temps nécessaire sous chauffage conventionnel.This study focuses on the synthesis and preparation of modified zeolites with transition metals and theirs applications in catalysis under microwave irradiation. Previous works have shown interest in modifying zeolites with transition metals for their application to oxidation reactions and in using microwave irradiation in order to increase the reaction rates. In this thesis, we studied two types of zeolite structure (MEL and FAU) doped with transitionmetals (Co, Mn, Fe, Zn, Ni, Cr) at different concentrations. A classic characterization study has increased the knowledge on the preparation of modified zeolites and the understanding of their influence on thecatalytic activity. The styrene partial oxidation reaction for benzaldehyde production was chosen as amodel reaction. Co-ZSM-11 zeolite presented the best catalytic activity in this study and also compared to other catalysts found in the literature. The styrene oxidation reactions were studied under microwave irradiation and under conventional heating. No difference in the activity of doped zeolites was observed for both types of heating. The low values of permittivity and permeability of zeolites doped with transition metals make difficult the intensification of the benzaldehyde production process from styrene oxidation under microwave. The parameters of the model reaction have been optimized and a reaction kinetic study was carried out by using the Co-ZSM-11 zeolite. Finally, the hysteresis dielectric heating was used in the synthesis of ZSM-11. The synthesis time was significantly reduced (80%) under microwave irradiation compared to conventional heating.ROUEN-INSA Madrillet (765752301) / SudocSudocFranceF

Síntesis y Caracterización de Zeolitas Mel y Fau Dopadas con Metales de Transición para su Aplicación a la Química Fina bajo Irradiación Microondas

The aim of this work is to obtain zeolites doped with transition metals for their application to the synthesis of chemical compounds under microwave.Microporous zeolites were modified with transition metals. Their crystal structures were verified by XRD. Their specific surfaces were determined by the BET method. The dielectric properties of compacted zeolites were measured using a reflection method. The temperature profiles of these compacted beds were determined under microwave irradiation. Heating phenomena in zeolites were interpreted using a modified Debye model. Lewis and Brönsted acid sites were quantified, and so their acid strength by FTIR of zeolites, after adsorption and desorption of pyridine. Finally, we evaluated the catalytic activity of zeolites in the partial oxidation of styrene, in a batch system, under classical and dielectric heating.El trabajo tiene como objetivo la obtención de zeolitas dopadas con metales de transición para su aplicación a la síntesis de compuestos químicos bajo microondas.Se modificaron zeolitas microporosas con metales de transición. Su estructura cristalina se verificó mediante XRD. Por el método BET se determinó el área superficial de cada zeolita. Por medio de un método de reflexión se midieron las propiedades dieléctricas de las zeolitas compactadas. Se determinaron los perfiles de temperatura de estos lechos zeolíticos compactados con calentamiento dieléctrico. Se interpretaron los fenómenos de calentamiento presentes en las zeolitas mediante el uso del modelo de Debye modificado. Se cuantificaron los sitios ácidos de Lewis y Brönsted y su fuerza ácida mediante FTIR de zeolitas luego de los procesos de adsorción y desorción de piridina. Finalmente, se evaluó la actividad catalítica de zeolitas en la oxidación parcial de estireno, en un sistema batch bajo calentamiento clásico y dieléctrico

Synthesis and characterization of MEL and FAU zeolites doped with transition metals for their application to the fine chemistry under microwave irradiation

International audienceDoped zeolites with transition metals were prepared for their application to the synthesis of chemical compounds under microwave irradiation. The zeolite crystalline structures were verified by XRD. Their surface areas were determined by the BET method. Lewis and Brönsted acid sites were quantified by FTIR of adsorbed pyridine in zeolites. The characterization of acidic properties revealed the generation of new Lewis acid sites after transition metal incorporation into zeolites. The dielectric properties of compacted zeolites were measured by using a reflection method. The temperature profiles of these compacted beds were measured during heating under microwave irradiation. Heating phenomena in zeolites were interpreted using a modified Debye model. Two main dielectric mechanisms were determined in zeolites: rotational polarization phenomenon and interfacial polarization. The selective catalytic oxidation of styrene with hydrogen peroxide was studied over zeolites doped with transition metals in a batch system, under conventional and microwave heating. Benzaldehyde was the main product in all the samples under study. Styrene conversion showed an important influence of the transition metal nature and content and so, the kind of zeolite structure used. With the present experimental conditions, no difference was proved between microwave and conventional heating neither on activity nor on selectivity