@misc{GonzalezAriasGonzalezCastanoSanchezetal., author = {Gonz{\´a}lez-Arias, Judith and Gonz{\´a}lez-Casta{\~n}o, Miriam and S{\´a}nchez, Marta Elena and Cara-Jim{\´e}nez, Jorge and Arellano-Garc{\´i}a, Harvey}, title = {Valorization of biomass-derived CO2 residues with Cu-MnOx catalysts for RWGS reaction}, series = {Renewable Energy}, journal = {Renewable Energy}, number = {182}, issn = {1879-0682}, doi = {10.1016/j.renene.2021.10.029}, pages = {443 -- 451}, abstract = {This study delivers useful understanding towards the design of effective catalytic systems for upgrading real CO2erich residual streams derived from biomass valorization. Within this perspective, a catalysts' series based on (5 wt\%) Cu - (X wt\%) Mn/Al2O3with X¼0, 3, 8, and 10 is employed. The improved catalyst performance achieved through Mn incorporation is ascribed to enhanced Cu dispersions and promoted surface basic concentrations. Under standard RWGS conditions, the highest reaction rates achieved by(5 wt\%) Cu - (8 wt\%) Mn/Al2O3catalyst were associated to improved Cu dispersions along with the constitution of highly active Cu-MnOxdomains. Remarkably, variations on the optimal Cu to Mn ratios were detected as a function of the RWGS reaction conditions. Thus, under simulated CO2-rich residual feedstock's, i.e., in presence of CO and CH4, the further promotion on the Cu dispersion attained by the larger amounts of MnOxrendered the (5 wt\%) Cu - (10 wt\%) Mn/Al2O3catalyst as the best performing sample. Overall, the presented outcomes underline operative strategies for developing catalytic systems with advanced implementation potentialities.}, language = {en} } @misc{GonzalezAriasBaenaMorenoGonzalezCastanoetal., author = {Gonz{\´a}lez-Arias, Judith and Baena-Moreno, Francisco Manuel and Gonz{\´a}lez-Casta{\~n}o, Miriam and Arellano-Garc{\´i}a, Harvey}, title = {Economic approach for CO2 valorization from hydrothermal carbonization gaseous streams via reverse water-gas shift reaction}, series = {Fuel}, volume = {313}, journal = {Fuel}, issn = {0016-2361}, doi = {10.1016/j.fuel.2021.123055}, pages = {1 -- 7}, abstract = {In this work the economic performance of valorizing the gaseous stream coming from hydrothermal carbonization (HTC) of olive tree pruning is presented as a novel strategy to improve the competitiveness of HTC. The valorization of the commonly disregarded gaseous stream produced in this thermochemical treatment was proposed via the Reverse Water-Gas Shift reaction. This allows to obtain syngas for selling and therefore improving the overall economic performance of the process. To this end, three plant sizes were selected (312.5, 625 and 1250 kg/h of biomass processing). The parameters with a higher share in the total cost distribution along with the revenues from the hydrochar and the syngas selling were further evaluated. The results evidenced that with the assumptions taken, the overall process is still not profitable. To reach profitability, syngas selling prices between 2.2 and 3.4 €/m3 are needed, revealing that this proposal is not economically attractive. Alternatively, a lack of competitiveness in the current market is revealed with hydrochar selling prices between 0.41 and 0.64 €/kg to make the project profitable. The catalyst cost, sharing approximately 20\% of the total cost, is the parameter with the highest impact in the total economics of the process. The second one is the hydrogen price production, representing almost 16\% of the total. Investment subsidies are also examined as a potential tool to cover part of the initial investment. These results evidenced that further efforts and measures are needed to push forward in the path towards circular economy societies.}, language = {en} } @misc{TarifaGonzalezCastanoCazanaetal., author = {Tarifa, Pilar and Gonz{\´a}lez-Casta{\~n}o, Miriam and Caza{\~n}a, F. and Monz{\´o}n, Antonio and Arellano-Garc{\´i}a, Harvey}, title = {Development of one-pot Cu/cellulose derived carbon catalysts for RWGS reaction}, series = {Fuel}, volume = {Vol. 319}, journal = {Fuel}, issn = {0016-2361}, doi = {10.1016/j.fuel.2022.123707}, pages = {7}, abstract = {A series of Cu-based catalysts promoted with Fe, Ce and Al supported on cellulose derived carbon (CDC) was prepared by biomorphic mineralization technique for the RWGS reaction. The excellent Cu dispersions (7 nm at ca. 30 wt\% Cu) along with the resilience toward metal sintering attained in the entire catalysts series highlight one-pot decomposition of cellulose under reducing atmosphere as an excellent synthesis method which enable obtaining well-dispersed Cu nanoparticles. The influence of incorporating a second metal oxide over biomorphic mineralized Cu systems was also investigated. With the Cu-Ce system exhibiting the best catalyst performance of the catalysts' series, the enhanced catalyst performances were majorly ascribed to the catalysts redox properties. The lineal relationships stablished between oxygen exchange capacity and CO2 conversion rates remarks the employed sequential H2/CO2 cycles as an effective methodology for screening the catalytic performance of Cu catalysts for RWGS reaction.}, language = {en} } @misc{MahmoodGonzalezCastanoPenkovaetal., author = {Mahmood, Safdar and Gonz{\´a}lez-Casta{\~n}o, Miriam and Penkova, Anna and Centeno, Miguel Angel and Odriozola, Jos{\´e} Antonio and Arellano-Garc{\´i}a, Harvey}, title = {CO2 methanation on Ni/YMn1-xAlxO3 perovskite catalysts}, series = {Applied Materials Today}, volume = {29}, journal = {Applied Materials Today}, issn = {2352-9407}, doi = {10.1016/j.apmt.2022.101577}, pages = {1 -- 11}, abstract = {Seeking for advanced catalytic systems for the CO2 methanation reaction, the use of Ni supported catalysts over redox materials is often proposed. Profiting the superior redox properties described for layered perovskite systems, this work has investigated a series Ni supported YMn1-xAlxO3 (x = 0, 0.2, 0.5, 0.8, 1) perovskite catalysts. The obtained results evidenced the impact of the support nature on the systems redox properties and Ni-support interactions. Within the catalysts series, the greater methanation rates displayed by Ni/YMn0.5Al0.5O3 catalyst (0.748 mmolCO2,conv.s-1 gNi -1 at 400 ◦C and 60 L/gh) were associated to the interplay between the support redox properties and superior Ni dispersion. The improved redox behavior attained through the Al-incorporation (up to x = 0.5) was associated to the layered perovskite structures which, being distorted and constituted by smaller crystal sizes, facilitated the behavior of Mn redox couples as surface species readily interconverted. Exhibiting catalytic performances comparable to precious metals based catalysts, this work proposes the Ni/YMn0.5Al0.5O3 catalyst as an effective system for the CO2 methanation reaction.}, language = {en} } @misc{GonzalezCastanoBaenaMorenoNavarrodeMigueletal., author = {Gonz{\´a}lez-Casta{\~n}o, Miriam and Baena-Moreno, Francisco Manuel and Navarro de Miguel, Juan Carlos and Miah, Kamal Uddin Mohammad and Arroyo-Torralvo, F{\´a}tima and Ossenbrink, Ralf and Odriozola, Jos{\´e} Antonio and Benzinger, Walther and Hensel, Andreas and Wenka, Achim and Arellano-Garc{\´i}a, Harvey}, title = {3D-printed structured catalysts for CO2 methanation reaction: Advancing of gyroid-based geometries}, series = {Energy Conversion and Management}, volume = {258}, journal = {Energy Conversion and Management}, issn = {2590-1745}, doi = {10.1016/j.enconman.2022.115464}, pages = {8}, abstract = {This work investigates the CO2 methanation rate of structured catalysts by tuning the geometry of 3D-printed metal Fluid Guiding Elements (FGEs) structures based on periodically variable pseudo-gyroid geometries. The enhanced performance showed by the structured catalytic systems is mostly associated with the capability of the FGEs substrate geometries for efficient heat usages. Thus, variations on the channels diameter resulted in ca. 25\% greater CO2 conversions values at intermediate temperature ranges. The highest void fraction evidenced in the best performing catalyst (3D-1) favored the radial heat transfer and resulted in significantly enhanced catalytic activity, achieving close to equilibrium (75\%) conversions at 400 ◦C and 120 mL/min. For the 3D-1 catalyst, a mathematical model based on an experimental design was developed thus enabling the estimation of its behavior as a function of temperature, spatial velocity, hydrogen to carbon dioxide (H2/CO2) ratio, and inlet CO2 concentration. Its optimal operating conditions were established under 3 different scenarios: 1) no restrictions, 2) minimum H2:CO2 ratios, and 3) minimum temperatures and H2/CO2 ratio. For instance, for the lattest scenario, the best CO2 methanation conditions require operating at 431 ◦C, 200 mL/min, H2/CO2 = 3 M ratio, and inlet CO2 concentration = 10 \%.}, language = {en} } @misc{MedinaMendezGonzalezCastanoBaenaMorenoetal., author = {Medina M{\´e}ndez, Juan Ali and Gonz{\´a}lez-Casta{\~n}o, Miriam and Baena-Moreno, Francisco Manuel and Arellano-Garc{\´i}a, Harvey}, title = {CO2 methanation: on the modeling of reacting laminar flows in structured Ni/MgAl2O4 catalysts}, series = {XXV Fluid Mechanics Conference, Rzesz{\´o}w, Poland, 7-9 September 2022, Book of Abstracts}, journal = {XXV Fluid Mechanics Conference, Rzesz{\´o}w, Poland, 7-9 September 2022, Book of Abstracts}, editor = {Kmiotek, M. and Kordos, A.}, publisher = {Publishing House of Rzesz{\´o}w University of Technology}, address = {Rzesz{\´o}w, Poland}, isbn = {978-83-7934-590-8}, pages = {98 -- 100}, language = {en} } @misc{MedinaMendezGonzalezCastanoBaenaMorenoetal., author = {Medina M{\´e}ndez, Juan Ali and Gonz{\´a}lez-Casta{\~n}o, Miriam and Baena-Moreno, Francisco Manuel and Arellano-Garc{\´i}a, Harvey}, title = {CO2 methanation: on the modeling of reacting laminar flows in structured Ni/MgAl2O4 catalysts}, series = {Journal of Physics: Conference Series}, journal = {Journal of Physics: Conference Series}, number = {2367}, publisher = {IOP Publishing}, doi = {10.1088/1742-6596/2367/1/012015}, pages = {8}, language = {en} } @misc{MiahKloshekGonzalezCastanoetal., author = {Miah, Kamal Uddin Mohammad and Kloshek, Alexander and Gonz{\´a}lez-Casta{\~n}o, Miriam and Kehm, Christian and Ossenbrink, Ralf and Michailov, Vesselin}, title = {Herstellen hocheffektiver Mikroreaktoren durch selektives Laserstrahlschmelzen}, series = {DVS Congress 2022, Große Schweißtechnische Tagung, DVS Campus ; Kurzfassungen der Vortr{\"a}ge der Veranstaltung in Koblenz vom 19. bis 21. September 2022 ; (Langfassungen der Beitr{\"a}ge auf USB-Karte)}, journal = {DVS Congress 2022, Große Schweißtechnische Tagung, DVS Campus ; Kurzfassungen der Vortr{\"a}ge der Veranstaltung in Koblenz vom 19. bis 21. September 2022 ; (Langfassungen der Beitr{\"a}ge auf USB-Karte)}, publisher = {DVS Media GmbH}, address = {D{\"u}sseldorf}, isbn = {978-3-96144-189-1}, pages = {708 -- 713}, abstract = {Das pulverbasierte 3D-Metalldrucken erm{\"o}glicht die Fertigung von hochkomplexen Integralbauteilen, die als Tr{\"a}gerstruktur f{\"u}r Mikroreaktoren benutzt werden. Nach einer Beschichtung der Struktur mit einem Katalysatormaterial, k{\"o}nnen diese Mikroreaktoren h{\"o}chst effizient f{\"u}r die CO2-Methanisierung eingesetzt werden. Durch die additive Fertigung mit dem selektiven Laserstrahlschmelzen (SLM) wurden adaptierte dreidimensionale periodische Gitterstrukturen mit sehr geringen Wandst{\"a}rken hergestellt. Diese weisen ein sehr g{\"u}nstiges Verh{\"a}ltnis von Oberfl{\"a}che zu Volumen (TPMS - Triply periodic minimal surface) auf. Des Weiteren zeigen die TPMS-Strukturen vorteilhafte Str{\"o}mungseigenschaften, die sowohl f{\"u}r die Beschichtung mit dem Katalysator-Material als auch die Durchstr{\"o}mung mit den Reaktionsmedien im Betrieb essentiell sind. So ist es beispielsweise m{\"o}glich, durch die Variation der Dimension einer TPMS-Struktur die Oberfl{\"a}che pro Volumeneinheit, den hydraulischen Durchmesser des Reaktors und somit auch den Transportprozess des Fluids deutlich zu verbessern. Diese Faktoren erm{\"o}glichen eine effektivere Gas-Katalysator-Reaktion. Im Vergleich zu Mikroreaktorstrukturen aus den traditionellen Herstellungsverfahren liefern die additiv gefertigten Strukturen sowohl eine h{\"o}here CO2-Umwandlungsrate als auch eine CH4-Selektivit{\"a}t innerhalb des diffusionskontrollierten Bereichs.}, language = {de} } @misc{TarifaRamirezReinaGonzalezCastanoetal., author = {Tarifa, Pilar and Ramirez Reina, Tomas and Gonz{\´a}lez-Casta{\~n}o, Miriam and Arellano-Garc{\´i}a, Harvey}, title = {Catalytic Upgrading of Biomass-Gasification Mixtures Using Ni-Fe/MgAl₂O₄ as a Bifunctional Catalyst}, series = {Energy and Fuels}, volume = {36}, journal = {Energy and Fuels}, number = {15}, issn = {1520-5029}, doi = {10.1021/acs.energyfuels.2c01452}, pages = {8267 -- 8273}, abstract = {Biomass gasification streams typically contain a mixture of CO, H2, CH4, and CO2 as the majority components and frequently require conditioning for downstream processes. Herein, we investigate the catalytic upgrading of surrogate biomass gasifiers through the generation of syngas. Seeking a bifunctional system capable of converting CO2 and CH4 to CO, a reverse water gas shift (RWGS) catalyst based on Fe/MgAl2O4 was decorated with an increasing content of Ni metal and evaluated for producing syngas using different feedstock compositions. This approach proved efficient for gas upgrading, and the incorporation of adequate Ni content increased the CO content by promoting the RWGS and dry reforming of methane (DRM) reactions. The larger CO productivity attained at high temperatures was intimately associated with the generation of FeNi3 alloys. Among the catalysts' series, Ni-rich catalysts favored the CO productivity in the presence of CH4, but important carbon deposition processes were noticed. On the contrary, 2Ni-Fe/MgAl2O4 resulted in a competitive and cost-effective system delivering large amounts of CO with almost no coke deposits. Overall, the incorporation of a suitable realistic application for valorization of variable composition of biomass-gasification derived mixtures obtaining a syngas-rich stream thus opens new routes for biosyngas production and upgrading.}, language = {en} } @misc{BobadillaAzancotLuqueAlvarezetal., author = {Bobadilla, Luis F. and Azancot, Lola and Luque-Alvarez, Ligia A. and Torres-Sempere, Guillermo and Gonzalez-Castano, Miriam and Pastor-Perez, Laura and Yu, Jie and Ramirez Reina, Tomas and Ivanova, Svetlana and Centeno, Miguel Angel and Odriozola, Jos{\´e} Antonio}, title = {Development of Power-to-X Catalytic Processes for CO2 Valorisation: From the Molecular Level to the Reactor Architecture}, series = {Chemistry}, volume = {4}, journal = {Chemistry}, number = {4}, issn = {2624-8549}, doi = {10.3390/chemistry4040083}, pages = {1250 -- 1280}, abstract = {Nowadays, global climate change is likely the most compelling problem mankind is facing. In this scenario, decarbonisation of the chemical industry is one of the global challenges that the scientific community needs to address in the immediate future. Catalysis and catalytic processes are called to play a decisive role in the transition to a more sustainable and low-carbon future. This critical review analyses the unique advantages of structured reactors (isothermicity, a wide range of residence times availability, complex geometries) with the multifunctional design of efficient catalysts to synthesise chemicals using CO2 and renewable H2 in a Power-to-X (PTX) strategy. Fine-chemistry synthetic methods and advanced in situ/operando techniques are essential to elucidate the changes of the catalysts during the studied reaction, thus gathering fundamental information about the active species and reaction mechanisms. Such information becomes crucial to refine the catalyst's formulation and boost the reaction's performance. On the other hand, reactors architecture allows flow pattern and temperature control, the management of strong thermal effects and the incorporation of specifically designed materials as catalytically active phases are expected to significantly contribute to the advance in the valorisation of CO2 in the form of high added-value products. From a general perspective, this paper aims to update the state of the art in Carbon Capture and Utilisation (CCU) and PTX concepts with emphasis on processes involving the transformation of CO2 into targeted fuels and platform chemicals, combining innovation from the point of view of both structured reactor design and multifunctional catalysts development.}, language = {en} }