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1. Operando X-ray Absorption Spectroscopy Investigation of Photocatalytic Hydrogen Evolution over Ultradispersed Pt/TiO 2 Catalysts

Author

C. Dessal, Olivier Proux, Jean-Luc Rousset, Yufen Chen, Jordi Llorca, Frederic Bourgain, Mimoun Aouine, Pavel Afanasiev, Lluís Soler, Laurent Piccolo, Thomas Len, Franck Morfin, Antonio Aguilar-Tapia, IRCELYON-Catalyse Hétérogène pour la Transition Energétique (CATREN), Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), IRCELYON-Ingéniérie, du matériau au réacteur (ING), Universitat Politècnica de Catalunya. Institut de Tècniques Energètiques, Universitat Politècnica de Catalunya. Departament d'Enginyeria Química, and Universitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia

Subjects
Materials science, XAS, Fotocatàlisi, Single-atom catalysis, Operando spectroscopy, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Catalysis, Pt/TiO2, Enginyeria química [Àrees temàtiques de la UPC], XAS 2, Photocatalytic hydrogen production, [CHIM]Chemical Sciences, Hydrogen evolution, Photocatalysis, Oxygenate, Hydrogen production, X-ray absorption spectroscopy, 010405 organic chemistry, General Chemistry, Hidrogen, [CHIM.CATA]Chemical Sciences/Catalysis, 0104 chemical sciences, Chemical engineering, Particle, Enginyeria química::Química física [Àrees temàtiques de la UPC], Hydrogen
Abstract

International audience; Photocatalytic hydrogen production from water or oxygenates is foreseen as a sustainable energy production route. In spite of recent performance achievements through Pt particle downsizing, the knowledge on the prototypical Pt/TiO 2 photocatalyst operation mechanism, in particular the electronic state and the stability of the Pt phase under reaction conditions, remains limited. We have investigated atomically dispersed Pt/TiO 2 catalysts by pre/post-reaction scanning transmission electron microscopy and operando X-ray absorption spectroscopy-mass spectrometry in gas-phase ethanol dehydrogenation conditions under ultraviolet-visible light irradiation. The catalysts were prepared by a simple impregnation method on two types of commercial titania. While the general effect of the reaction on initially fully oxidized (Pt IV) single-atom catalysts (SACs) is Pt reduction and aggregation, this combined phenomenon can be inhibited in two manners. First, when supported on high-surface-area anatase, the Pt SAC retains an intermediate oxidation state, and its clustering is limited to Pt dimers and trimers. Second, with the same support, a mild reducing pretreatment generates, through the formation of Pt-Ti bonds, near-neutral and ultradispersed Pt species (from single atoms to nanometric clusters) with the highest stability and activity in photocatalytic hydrogen evolution.

Published
2020

2. Remarkable Carbon Dioxide Hydrogenation to Ethanol on a Palladium/Iron Oxide Single-Atom Catalyst

Author

Laurent Piccolo, Jordi Llorca, Marta D. Rossell, Francisco J. Caparrós, Lluís Soler, Inmaculada Angurell, Oriol Rossell, IRCELYON-Catalyse Hétérogène pour la Transition Energétique (CATREN), Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Universitat Politècnica de Catalunya. Institut de Tècniques Energètiques, Universitat Politècnica de Catalunya. Departament d'Enginyeria Química, and Universitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia

Subjects
Palladium compounds, Materials science, Inorganic chemistry, Catalitzadors, Iron oxide, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, Indústria química, 01 natural sciences, 7. Clean energy, Catalysis, Inorganic Chemistry, chemistry.chemical_compound, Enginyeria química [Àrees temàtiques de la UPC], Catàlisi, Physical and Theoretical Chemistry, Pal·ladi--Compostos, Ethanol, Catalysts, Organic Chemistry, Atom (order theory), [CHIM.CATA]Chemical Sciences/Catalysis, 021001 nanoscience & nanotechnology, [SDE.ES]Environmental Sciences/Environmental and Society, 0104 chemical sciences, chemistry, Enginyeria química::Impacte ambiental [Àrees temàtiques de la UPC], 13. Climate action, Carbon dioxide, 0210 nano-technology, Enginyeria química::Indústries químiques [Àrees temàtiques de la UPC], Palladium, Chemical industry
Abstract

The hydrogenation of CO2 into value-added chemicals is one of the most investigated methods to reduce CO2 emissions in the atmosphere and thereby contributes to a sustainable chemical industry. Whereas the catalytic hydrogenation of CO2 into methanol and synthetic hydrocarbons is well established, the effective and selective transformation of CO2 into higher alcohols is still challenging. Here, we show that Pd single atoms anchored on the surface of Fe3O4 are very active for the hydrogenation of CO2 to ethanol at 300 8C, even at atmospheric pressure. By comparing various Pd/MOx catalysts, we conclude that the metal–oxide interface has a strong influence on catalytic behavior.

Published
2018

3. A plausible link between the asteroid 21 Lutetia and CH carbonaceous chondrites

Author

Albert Rimola, M. A. Barucci, Carles E. Moyano-Cambero, Sonia Fornasier, Jordi Llorca, Josep M. Trigo-Rodríguez, Universitat Politècnica de Catalunya [Barcelona] (UPC), Laboratoire d'études spatiales et d'instrumentation en astrophysique (LESIA), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), departament de Quimica, Universitat Autònoma de Barcelona (UAB), Universitat Politècnica de Catalunya. Departament d'Enginyeria Química, and Universitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia

Subjects
Asteroides, Physics and chemistry in space. Planetology, 010504 meteorology & atmospheric sciences, Planetologia, FOS: Physical sciences, Aeròlits, 01 natural sciences, Parent body, Astrobiology, Enginyeria química [Àrees temàtiques de la UPC], Chondrite, 0103 physical sciences, 010303 astronomy & astrophysics, 0105 earth and related environmental sciences, Earth and Planetary Astrophysics (astro-ph.EP), Thermal infrared, [SDU.ASTR]Sciences of the Universe [physics]/Astrophysics [astro-ph], Meteoroids, Asteroids, Geophysics, Planetary science, Meteorite, Space and Planetary Science, Asteroid, [SDU]Sciences of the Universe [physics], Carbonaceous chondrite, Geology, Astrophysics - Earth and Planetary Astrophysics
Abstract

A crucial topic in planetology research is establishing links between primitive meteorites and their parent asteroids. In this study we investigate the feasibility of a connection between asteroids similar to 21 Lutetia, encountered by the Rosetta mission in July 2010, and the CH3 carbonaceous chondrite Pecora Escarpment 91467 (PCA 91467). Several spectra of this meteorite were acquired in the ultraviolet to near-infrared (0.3 to 2.2 {\mu}m) and in the mid-infrared to thermal infrared (2.5 to 30.0 {\mu}m or 4000 to ~333 cm^-1), and they are compared here to spectra from the asteroid 21 Lutetia. There are several similarities in absorption bands and overall spectral behavior between this CH3 meteorite and 21 Lutetia. Considering also that the bulk density of Lutetia is similar to that of CH chondrites, we suggest that this asteroid could be similar, or related to, the parent body of these meteorites, if not the parent body itself. However, the apparent surface diversity of Lutetia pointed out in previous studies indicates that it could simultaneously be related to other types of chondrites. Future discovery of additional unweathered CH chondrites could provide deeper insight in the possible connection between this family of metal-rich carbonaceous chondrites and 21 Lutetia or other featureless, possibly hydrated high-albedo asteroids., Comment: 26 pages, 7 figures and 2 tables, Meteoritics and Planetary Science, manuscript #2225 (2016)

Published
2016

4. Monte carlo simulations of the n_TOF lead spallation target with the Geant4 toolkit: A benchmark study

Author

S. Warren, J. Andrzejewski, V. Variale, M. Mastromarco, Pedro G. Ferreira, G. Vannini, M. A. Cortés-Giraldo, Rugard Dressler, N. Patronis, A. K. Saxena, Arnaud Ferrari, J. Billowes, J. Marganiec, E. Jericha, Paolo Finocchiaro, Anton Wallner, M. Caamaño, Nicola Colonna, A. Musumarra, Dorothea Schumann, E. Chiaveri, P. F. Mastinu, J. Balibrea, J. A. Ryan, Vasilis Vlachoudis, C. Rubbia, A. Tarifeño-Saldivia, G. Cortes, E. González, A. Pavlik, L. Audouin, A. Ventura, M. Sabaté-Gilarte, F. Calviño, H. Leeb, J. Perkowski, A. Casanovas, Y. H. Chen, P. C. Rout, C. Domingo-Pardo, M. Bacak, A. Kimura, J. L. Tain, F. Gunsing, T. Glodariu, F. Mingrone, A. Masi, D. G. Jenkins, E. Dupont, Cristian Massimi, C. Lederer, M. Diakaki, Niko Kivel, F. Cerutti, M. Krtička, Kathrin Göbel, A. S. Brown, Alexandru Negret, S. J. Lonsdale, J. Lerendegui-Marco, E. Mendoza, T. Martinez, B. Fernández-Domínguez, F. Käppeler, Jan Heyse, Mario Barbagallo, M.B. Gómez-Hornillos, A. Oprea, A. Kalamara, I. F. Gonçalves, Javier Praena, S. Lo Meo, P. M. Milazzo, A. Stamatopoulos, S. Heinitz, Ignacio Porras, F. Bečvář, T. J. Wright, D. Mancussi, Simone Gilardoni, Hideo Harada, Rene Reifarth, R. Cardella, A. Mengoni, O. Aberle, Peter Schillebeeckx, J. M. Quesada, L. Tassan-Got, Deniz Kurtulgil, R. Vlastou, P. Vaz, D. Radeck, E. Berthoumieux, L. Cosentino, N. V. Sosnin, Annamaria Mazzone, Petar Žugec, D. Bosnar, D. Macina, Carlos Guerrero, G. Tagliente, D. Cano-Ott, Y. Kadi, S. Valenta, Marco Calviani, A. G. Smith, Philip Woods, A. R. García, Emilio Andrea Maugeri, M. Kokkoris, E. Leal-Cidoncha, A. Gawlik, Thomas Rauscher, I. Duran, P. Kavrigin, Ralf Nolte, E. Griesmayer, L. A. Damone, Institut de Recherches sur les lois Fondamentales de l'Univers (IRFU), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, Institut de Physique Nucléaire d'Orsay (IPNO), Université Paris-Sud - Paris 11 (UP11)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Centre National de la Recherche Scientifique (CNRS), n_TOF, Lerendegui-Marco, J., Cortés-Giraldo, M.A., Guerrero, C., Quesada, J.M., Meo, S. Lo, Massimi, C., Barbagallo, M., Colonna, N., Mancussi, D., Mingrone, F., Sabaté-Gilarte, M., Vannini, G., Vlachoudis, V., Aberle, O., Andrzejewski, J., Audouin, L., Bacak, M., Balibrea, J., Bečvář, F., Berthoumieux, E., Billowes, J., Bosnar, D., Brown, A., Caamaño, M., Calviño, F., Calviani, M., Cano-Ott, D., Cardella, R., Casanovas, A., Cerutti, F., Chen, Y.H., Chiaveri, E., Cortés, G., Cosentino, L., Damone, L.A., Diakaki, M., Domingo-Pardo, C., Dressler, R., Dupont, E., Durán, I., Fernández-Domínguez, B., Ferrari, A., Ferreira, P., Finocchiaro, P., Göbel, K., Gómez-Hornillos, M.B., García, A.R., Gawlik, A., Gilardoni, S., Glodariu, T., Gonçalves, I.F., González, E., Griesmayer, E., Gunsing, F., Harada, H., Heinitz, S., Heyse, J., Jenkins, D.G., Jericha, E., Käppeler, F., Kadi, Y., Kalamara, A., Kavrigin, P., Kimura, A., Kivel, N., Kokkoris, M., Krtička, M., Kurtulgil, D., Leal-Cidoncha, E., Lederer, C., Leeb, H., Lonsdale, S.J., Macina, D., Marganiec, J., Martínez, T., Masi, A., Mastinu, P., Mastromarco, M., Maugeri, E.A., Mazzone, A., Mendoza, E., Mengoni, A., Milazzo, P.M., Musumarra, A., Negret, A., Nolte, R., Oprea, A., Patronis, N., Pavlik, A., Perkowski, J., Porras, I., Praena, J., Radeck, D., Rauscher, T., Reifarth, R., Rout, P.C., Rubbia, C., Ryan, J.A., Saxena, A., Schillebeeckx, P., Schumann, D., Smith, A.G., Sosnin, N.V., Stamatopoulos, A., Tagliente, G., Tain, J.L., Tarifeño-Saldivia, A., Tassan-Got, L., Valenta, S., Variale, V., Vaz, P., Ventura, A., Vlastou, R., Wallner, A., Warren, S., Woods, P.J., Wright, T., Ugec, P., Universitat Politècnica de Catalunya. Departament de Física, Universitat Politècnica de Catalunya. Institut de Tècniques Energètiques, Universitat Politècnica de Catalunya. ANT - Advanced Nuclear Technologies Research Group, Universitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia, Centre National de la Recherche Scientifique (CNRS)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Université Paris-Sud - Paris 11 (UP11), and Universidad de Sevilla. Departamento de Física Atómica, Molecular y Nuclear

Subjects
nTOF, [PHYS.NUCL]Physics [physics]/Nuclear Theory [nucl-th], QC1-999, Astrophysics::High Energy Astrophysical Phenomena, Montecarlo, Mètode de, Monte Carlo method, Context (language use), Neutron, 01 natural sciences, Nuclear physics, Physics and Astronomy (all), Informàtica [Àrees temàtiques de la UPC], Neutron flux, CERN, 0103 physical sciences, Spallation, 010306 general physics, Nuclear Experiment, Monte Carlo, Neutrons, Physics, Large Hadron Collider, Física [Àrees temàtiques de la UPC], 010308 nuclear & particles physics, Neutron radiation, Cascade, Nuclear Physics - Theory
Abstract

Monte Carlo (MC) simulations are an essential tool to determine fundamental features of a neutron beam, such as the neutron flux or the γ -ray background, that sometimes can not be measured or at least not in every position or energy range. Until recently, the most widely used MC codes in this field had been MCNPX and FLUKA. However, the Geant4 toolkit has also become a competitive code for the transport of neutrons after the development of the native Geant4 format for neutron data libraries, G4NDL. In this context, we present the Geant4 simulations of the neutron spallation target of the n TOF facility at CERN, done with version 10.1.1 of the toolkit. The first goal was the validation of the intra-nuclear cascade models implemented in the code using, as benchmark, the characteristics of the neutron beam measured at the first experimental area (EAR1), especially the neutron flux and energy distribution, and the time distribution of neutrons of equal kinetic energy, the so-called Resolution Function. The second goal was the development of aMonte Carlo tool aimed to provide useful calculations for both the analysis and planning of the upcoming measurements at the new experimental area (EAR2) of the facility., The research that led to these results has received funding from the EC FP7 Programme under the projects NEUTANDALUS (Grant No. 334315) and CHANDA (Grant No. 605203), and the Spanish Ministry of Economy and Competitiveness projects FPA2011-28770- C3-02, FPA2013-45083-P and FPA2014- 53290-C2-2-P. The simulations have been performed at the computing cluster FISATOM, hosted at CICA (Seville, Spain), and of INFN-CNAF, University of Bologna; we thank the staff of both institutions for the operational maintenance of the machines.

Published
2016

5. FIRST EURADOS INTERCOMPARISON EXERCISE OF EYE LENS DOSEMETERS FOR MEDICAL APPLICATIONS

Author

Filip Vanhavere, Eleftheria Carinou, Isabelle Clairand, L Van Rycheghem, J. Daures, Sara Principi, Edilaine Honorio da Silva, M. Denoziere, M Roig, Mercè Ginjaume, Institut de Radioprotection et de Sûreté Nucléaire (IRSN), Universitat Politècnica de Catalunya [Barcelona] (UPC), Belgian Nuclear Research Centre, Greek Atomic Energy Commission (EEAE), Laboratoire National Henri Becquerel (LNHB), Département Métrologie Instrumentation & Information (DM2I), Laboratoire d'Intégration des Systèmes et des Technologies (LIST (CEA)), Direction de Recherche Technologique (CEA) (DRT (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Technologique (CEA) (DRT (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire d'Intégration des Systèmes et des Technologies (LIST (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Département d'instrumentation Numérique (DIN (CEA-LIST)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Vrije Universiteit Brussel (VUB), European Project, Greek Atomic Energy Commission, Laboratoire d'Intégration des Systèmes et des Technologies (LIST), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire d'Intégration des Systèmes et des Technologies (LIST), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, Universitat Politècnica de Catalunya. Institut de Tècniques Energètiques, Universitat Politècnica de Catalunya. DRM - Dosimetria i Radiofísica Mèdica, Universitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia, and Faculty of Medicine and Pharmacy

Subjects
Ciències de la visió::Òptica física [Àrees temàtiques de la UPC], Radiation Dosimetry, Nuclear instrumentation, 030218 nuclear medicine & medical imaging, law.invention, 0302 clinical medicine, Radiation dosimetry, law, Medicine, media_common, Radiation, Radiological and Ultrasound Technology, thermoluminescent detector, General Medicine, phantom, 3. Good health, Europe, Lens (optics), intercomparison exercise, Radioactivity, 030220 oncology & carcinogenesis, Calibration, Ophthalmic lenses, Lents oftàlmiques, Occupational exposure, Dosemeter, Dosemeters, Ionizing radiation, eye lens dose, Context (language use), [SDV.IB.MN]Life Sciences [q-bio]/Bioengineering/Nuclear medicine, [PHYS.NEXP]Physics [physics]/Nuclear Experiment [nucl-ex], Radiation Dosage, Dose measurement, 03 medical and health sciences, Dose limit, Radiation Protection, Radiation Monitoring, Dosimetry, Lens, Crystalline, Humans, Física::Electromagnetisme [Àrees temàtiques de la UPC], media_common.cataloged_instance, Radiology, Nuclear Medicine and imaging, European Union, [PHYS.PHYS.PHYS-INS-DET]Physics [physics]/Physics [physics]/Instrumentation and Detectors [physics.ins-det], European union, Eye lens, Protocol (science), Photons, Física [Àrees temàtiques de la UPC], Radiation Dosimeters, business.industry, Public Health, Environmental and Occupational Health, occupational exposure, Radiació--Dosimetria, Optometry, Ciències de la visió [Àrees temàtiques de la UPC], business
Abstract

International audience; In the context of the decrease in the eye lens dose limit for occupational exposure to 20 mSv per year stated by the recent revision of the European Basic Safety Standards Directive 2013/59/EURATOM, the European Radiation Dosimetry Group (EURADOS) has organised in 2014, for the first time, an intercomparison exercise for eye lens dosemeters. The main objective was to assess the capabilities of the passive eye lens dosemeters currently in use in Europe for occupational monitoring in medical fields. A total of 20 European individual monitoring services from 15 different countries have participated. The dosemeters provided by the participants were all composed of thermoluminescent detectors, of various types and designs. The irradiations were carried out with several photon fields chosen to cover the energy and angle ranges encountered in medical workplace. Participants were asked to report the doses in terms of H-p(3) using their routine protocol. The results provided by each participant were compared with the reference delivered doses. All the results were anonymously analysed. Results are globally satisfactory since, among the 20 participants, 17 were able to provide 90 % of their response in accordance with the ISO 14146 standard requirements.

Published
2016

6. Experimental and exergy evaluation of ethanol catalytic steam reforming in a membrane reactor

Author

Jordi Llorca, Ali Hedayati, Olivier Le Corre, Bruno Lacarrière, Laboratoire de génie des procédés - environnement - agroalimentaire (GEPEA), Mines Nantes (Mines Nantes)-Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Ecole Nationale Vétérinaire, Agroalimentaire et de l'alimentation Nantes-Atlantique (ONIRIS)-Centre National de la Recherche Scientifique (CNRS), Mines Nantes (Mines Nantes), Universitat Politècnica de Catalunya [Barcelona] (UPC), Universitat Politècnica de Catalunya. Institut de Tècniques Energètiques, and Universitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia

Subjects
Exergy, [SPI.OTHER]Engineering Sciences [physics]/Other, Hydrogen, Energies [Àrees temàtiques de la UPC], Hydrogen as fuel, chemistry.chemical_element, Ethanol steam reforming, Física::Termodinàmica [Àrees temàtiques de la UPC], 02 engineering and technology, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Catalytic membrane reactor, Catalysis, Steam reforming, chemistry.chemical_compound, Bioreactors, Hidrogen com a combustible, Termodinàmica, Ethanol, Membrane reactor, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Membrane, chemistry, Chemical engineering, Exergy efficiency, Thermodynamics, Energies::Recursos energètics renovables [Àrees temàtiques de la UPC], 0210 nano-technology, Alcohol
Abstract

International audience; The application of exergy analysis in the evaluation of the ethanol steam reforming (ESR) process in a catalytic membrane reactor (CMR) was presented. ESR experiments were performed at T = 873–923 K and P = 4–12 bar in a CMR containing Pd–Ag membranes sandwiched by Pd–Rh/CeO2 catalyst, aiming to produce fuel cell grade pure hydrogen. The effect of the operating conditions on the pure hydrogen production rate, hydrogen yield and recovery, exergy efficiency, and thermodynamic losses was investigated. Total hydrogen yield of 3.5 mol H2 permeated per mol ethanol in feed with maximum hydrogen recuperation of 90% was measured at 923 K and 12 bar. The highest amount of exergy was destructed via heat losses and the retentate gas stream. Exergy efficiency up to around 50% was reached in the case of the insulated reactor at 12 bar and 923 K. Exergy efficiency placed between 70–90% in the case of recovery of the retentate gas in an insulated reactor. It was concluded that operating at the highest pressure, the lowest S/C ratio, and 923 K gives the best exergy efficiency.

Published
2016

7. Dynamic simulation of pure hydrogen production via ethanol steam reforming in a catalytic membrane reactor

Author

Bruno Lacarrière, Jordi Llorca, Olivier Le Corre, Ali Hedayati, Laboratoire de génie des procédés - environnement - agroalimentaire (GEPEA), Mines Nantes (Mines Nantes)-Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Ecole Nationale Vétérinaire, Agroalimentaire et de l'alimentation Nantes-Atlantique (ONIRIS)-Centre National de la Recherche Scientifique (CNRS), Mines Nantes (Mines Nantes), Universitat Politècnica de Catalunya. Departament d'Enginyeria Química, and Universitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia

Subjects
Hydrogen, Etanol, Membrane reactor, Thermodynamics, chemistry.chemical_element, Mechanical engineering, Ethanol steam reforming, 02 engineering and technology, 7. Clean energy, Catalysis, Industrial and Manufacturing Engineering, Isothermal process, Steam reforming, symbols.namesake, Enginyeria química [Àrees temàtiques de la UPC], Catàlisi, Simulació per ordinador, 0502 economics and business, [SPI.GPROC]Engineering Sciences [physics]/Chemical and Process Engineering, 050207 economics, Electrical and Electronic Engineering, Civil and Structural Engineering, Hydrogen production, Arrhenius equation, Ethanol, Ideal gas law, Mechanical Engineering, 05 social sciences, Hidrogen, Building and Construction, 021001 nanoscience & nanotechnology, Pollution, Dynamic simulation, General Energy, chemistry, symbols, Pure hydrogen production, Sieverts' law, 0210 nano-technology
Abstract

International audience; Ethanol steam reforming (ESR) was performed over Pd-Rh/CeO 2 catalyst in a catalytic membrane reactor (CMR) as a reformer unit for production of fuel cell grade pure hydrogen. Experiments were performed at 923 K, 6e10 bar, and fuel flow rates of 50e200 ml/min using a mixture of ethanol and distilled water with steam to carbon ratio of 3. A static model for the catalytic zone was derived from the Arrhenius law to calculate the total molar production rates of ESR products, i.e. CO, CO 2 , CH 4 , H 2 , and H 2 O in the catalytic zone of the CMR (coefficient of determination R 2 ¼ 0.993). The pure hydrogen production rate at steady state conditions was modeled by means of a static model based on the Sieverts' law. Finally, a dynamic model was developed under ideal gas law assumptions to simulate the dynamics of pure hydrogen production rate in the case of the fuel flow rate or the operating pressure set point adjustment (transient state) at isothermal conditions. The simulation of fuel flow rate change dynamics was more essential compared to the pressure change one, as the system responded much faster to such an adjustment. The results of the dynamic simulation fitted very well to the experimental values at P ¼ 7e10 bar, which proved the robustness of the simulation based on the Sieverts' law. The simulation presented in this work is similar to the hydrogen flow rate adjustments needed to set the electrical load of a fuel cell, when fed online by the pure hydrogen generating reformer studied.

Published
2016

8. Exergetic study of catalytic steam reforming of bio-ethanol over Pd-Rh/CeO2 with hydrogen purification in a membrane reactor

Author

Bruno Lacarrière, Jordi Llorca, Ali Hedayati, Olivier Le Corre, Laboratoire de génie des procédés - environnement - agroalimentaire (GEPEA), Mines Nantes (Mines Nantes)-Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Ecole Nationale Vétérinaire, Agroalimentaire et de l'alimentation Nantes-Atlantique (ONIRIS)-Centre National de la Recherche Scientifique (CNRS), Mines Nantes (Mines Nantes), Universitat Politècnica de Catalunya. Institut de Tècniques Energètiques, and Universitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia

Subjects
Exergy, Thermal efficiency, Energies [Àrees temàtiques de la UPC], Membrane reactor, Energies::Eficiència energètica [Àrees temàtiques de la UPC], Energy Engineering and Power Technology, Thermodynamics, 7. Clean energy, Hydrogen purifier, Catalysis, Steam reforming, [SPI]Engineering Sciences [physics], Bioreactors, Exergy efficiency, Termodinàmica, Renewable Energy, Sustainability and the Environment, Chemistry, Catalytic steam reforming, Condensed Matter Physics, Fuel Technology, Volume (thermodynamics), 13. Climate action, Exergy destruction, Enginyeria química::Química física [Àrees temàtiques de la UPC]
Abstract

International audience; An exergy analysis of the ethanol steam reforming process using a Pd-Rh catalyst supported on ceria in a Pd-Ag membrane reactor has been performed based on experimental data. Both chemical and physical exergy for chemical species together with thermodynamic loss calculations have been considered to evaluate the exergy efficiency of the process. The system has been studied under different operational conditions in terms of temperature (873-923 K), pressure (4-12 bar), and feed flow rate using a water ethanol mixture of 50-50% volume (S/C = 1.6). A significant exergy efficiency dependency on the fuel flow rate and pressure has been encountered when considering the heat loss from the reactor. The best results regarding the exergetic and thermal efficiency have been obtained at high flow rates and 8-12 bar, which has been attributed to the higher hydrogen permeation through the membrane. The chemical reactions involved in the reforming process and the heat losses are the main sources of exergy destruction. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.

Published
2015

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