The objective of the thesis work presented here was the experimental evaluation and kinetic modelling of three different Pt-based catalysts used in the Water-Gas-Shift reactor, as part of the development of a combined heat and power system for residential applications, within the MICROGEN30 project funded by the Industria 2015 program. The catalysts studied are Pt/CeO2/Al2O3 and Pt/CeO2/Al2O3 with the ionic conductor (Zr/Eu/Mo oxides), on a metallic monolith support, made and provided by Institute of Materials Science of Seville, Department of Inorganic Chemistry, Spain. The third catalyst tested was Pt-based commercial catalyst coated on a spherical support. All these are typically employed in small scale plants used in fuel processing applications. Experimental part of the work included investigation of the performance and stability of the catalysts when subjected to different reactant concentrations at the same operating conditions. Several experimental campaigns were made for each catalyst, to evaluate the effect of the inlet concentration of each species on the reaction. Due to the different geometries of the catalysts’ supports, the reactor configuration was slightly modified, to allow the proper assembly. Finally, using the collected experimental data, it was possible to develop several kinetic expressions to describe the studied systems. By performing low conversion data analysis, reaction orders with respect to different species were defined. Based on this information for each catalyst, kinetic expressions are modified, and their parameters evaluated to obtain the best possible agreement between the experimental data and the model predictions.
L’obiettivo del presente lavoro di tesi è la valutazione sperimentale e la modellazione cinetica di tre diversi catalizzatori a base Pt utilizzati nei reattori di Water Gas Shift, come parte dello sviluppo di un sistema di cogenerazione per applicazioni residenziali. Il lavoro si inquadra nel più ampio progetto nazionale denominato MICROGEN30, finanziato dal programma Industria 2015. I catalizzatori studiati sono Pt/CeO2/Al2O3 e Pt/CeO2/Al2O3 con conduttori ionici (ossidi di Zr/Eu/Mo), su un supporto metallico a forma di monolita, realizzati presso L’Istituto di Scienze dei Materiali di Siviglia, Dipartimento di Chimica Inorganica, Spagna. Il terzo catalizzatori testato è di tipo commerciale, a base Pt, disperso su un supporto sferico. Tutti questi catalizzatori sono generalmente impiegati in impianti di piccole dimensioni, principalmente per applicazioni di fuel processing. La parte sperimentale del lavoro ha riguardato lo studio delle prestazioni e della stabilità dei catalizzatori, sottoposti a flussi di reagenti e prodotti a diverse concentrazioni, alle stesse condizioni di lavoro. Diverse campagne sperimentali sono state realizzate per ciascun catalizzatore, per valutare l’effetto della concentrazione in ingresso di ciascuna specie sulla reazione. Data la diversa geometria dei supporti dei catalizzatori, la configurazione del reattore è stata leggermente modificata, per permetterne un corretto montaggio. Infine, utilizzando i dati sperimentali raccolti, è stato possibile sviluppare diverse espressioni cinetiche per descrivere i sistemi studiati. Tramite l’analisi dei dati a bassa conversione di CO, gli ordini di reazione rispetto alle diverse specie sono stati stimati. Basandosi su queste informazioni per ciascun catalizzatore, le espressioni cinetiche sono state dunque adattate caso per caso, valutandone i parametri in esse contenute per ottenere il migliore accordo possibile tra le predizioni del modello ed i dati sperimentali.
Kinetics of the water gas shift reaction over Pt-based catalysts for a combined heat and power system
ALEKSIC, JANA;PRODORUTTI, STEFANO
2016/2017
Abstract
The objective of the thesis work presented here was the experimental evaluation and kinetic modelling of three different Pt-based catalysts used in the Water-Gas-Shift reactor, as part of the development of a combined heat and power system for residential applications, within the MICROGEN30 project funded by the Industria 2015 program. The catalysts studied are Pt/CeO2/Al2O3 and Pt/CeO2/Al2O3 with the ionic conductor (Zr/Eu/Mo oxides), on a metallic monolith support, made and provided by Institute of Materials Science of Seville, Department of Inorganic Chemistry, Spain. The third catalyst tested was Pt-based commercial catalyst coated on a spherical support. All these are typically employed in small scale plants used in fuel processing applications. Experimental part of the work included investigation of the performance and stability of the catalysts when subjected to different reactant concentrations at the same operating conditions. Several experimental campaigns were made for each catalyst, to evaluate the effect of the inlet concentration of each species on the reaction. Due to the different geometries of the catalysts’ supports, the reactor configuration was slightly modified, to allow the proper assembly. Finally, using the collected experimental data, it was possible to develop several kinetic expressions to describe the studied systems. By performing low conversion data analysis, reaction orders with respect to different species were defined. Based on this information for each catalyst, kinetic expressions are modified, and their parameters evaluated to obtain the best possible agreement between the experimental data and the model predictions.| File | Dimensione | Formato | |
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Master Thesis - J. Aleksic S. Prodorutti.pdf
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https://hdl.handle.net/10589/138786