Browsing by Author "Di Felice, Luca"
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Item H2 production via ammonia decomposition in a catalytic membrane reactor(2021-06-01) Cechetto, Valentina; Di Felice, Luca; Medrano, Jose A.; Makhloufi, Camel; Zuniga, Jon; Gallucci, Fausto; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSThe membrane reactor is proposed in this work as a system with high potential to efficiently recover the hydrogen (H2) stored in ammonia (NH3), which has been recently proposed as an alternative for H2 storage. With this technology, NH3 decomposition and high-purity H2 separation are simultaneously performed within the same unit, and high H2 separation efficiency is achieved at lower temperature compared to conventional systems, leading to energetic and economic benefits. NH3 decomposition was experimentally performed in a Pd-based membrane reactor over a Ru-based catalyst and the performance of the conventional packed bed reactor were used as benchmark for a comparison. The results demonstrate that the introduction of a membrane in a conventional reactor enhances its performance and allows to achieve conversion higher than the thermodynamic equilibrium conversion for sufficiently high temperatures. For temperatures from and above 425 °C, full NH3 conversion was achieved and more than 86% of H2 fed to the system as ammonia was recovered with a purity of 99.998%. The application of vacuum at the membrane permeate side leads to higher H2 recovery and NH3 conversions beyond thermodynamic restrictions. On the other hand, the reactor feed flow rate and operating pressure have not shown major impacts on NH3 conversion.Item Kinetic model for Pd-based membranes coking/deactivation in propane dehydrogenation processes(Elsevier B.V., 2023-01-15) Brencio, Camilla; Gough, Robin; de Leeuw den Bouter, Anouk; Arratibel, Alba; Di Felice, Luca; Gallucci, FaustoThis work aims at providing insight into the deactivation mechanism of Pd-based membranes in propane dehydrogenation processes. Thermogravimetric analysis (TGA) experiments were conducted to study the adsorption and coking of propylene over conventional thin layer (TL) and double-skinned (DS) Pd-based membranes under several operating conditions. A mechanistic monolayer-multilayer coke growth model was selected to mathematically describe the membrane coking observed during TGA experiments. In addition, the reaction rate of coke formation and its influence on membranes deactivation has been studied. The deactivation model able to describe the hydrogen flux decay over time suggests that monolayer coke is the main responsible for the membrane deactivation. Multilayer coke also causes deactivation but with a smaller order than monolayer coke, for both the TL and the DS membranes. Among the two membrane types, DS membrane deactivates faster, i.e. with a higher order than the TL membrane, which is equal to 1.55 for the former and 0.51 for the latter. This is related to the higher number of active sites available in the controlling step of the deactivation reaction, which are most probably given by the addition of the ceramic Al2O3 protective layer. XPS spectra further confirms that, in the presence of Pd, Al2O3 sites contribute to carbon formation by evidencing a different nature of carbon formed on the two membranes. Finally, the experimental results of hydrogen permeation over time conducted on different membranes types and operative conditions confirmed the validity of the derived and parametrized kinetic models for coke formation and membrane deactivation. The experimental findings and the kinetic model derived in this work provide essential tools for the design and optimization of membrane reactors for dehydrogenation processes.Item Ultra-pure hydrogen production via ammonia decomposition in a catalytic membrane reactor(2022-06-08) Cechetto, Valentina; Di Felice, Luca; Gutierrez Martinez, Rocio; Arratibel Plazaola, Alba; Gallucci, Fausto; Tecnalia Research & Innovation; TECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOSIn this work two alternatives are presented for increasing the purity of hydrogen produced in a membrane reactor for ammonia decomposition. It is experimentally demonstrated that either increasing the thickness of the membrane selective layer or using a small purification unit in the permeate of the membranes, ultra-pure hydrogen can be produced. Specifically, the results show that increasing the membrane thickness above 6 μm ultra-pure hydrogen can be obtained at pressures below 5 bar. A cheaper solution, however, consists in the use of an adsorption bed downstream the membrane reactor. In this way, ultra-pure hydrogen can be achieved with higher reactor pressures, lower temperatures and thinner membranes, which result in lower reactor costs. A possible process diagram is also reported showing that the regeneration of the adsorption bed can be done by exploiting the heat available in the system and thus introducing no additional heat sources.