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Browsing ENERGIA by Author "Abanades, Stéphane"
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- 3DOM ceria ecoceramics from sustainable cork templates for solar thermochemical CO2 splittingPublication . Pullar, Robert C.; Novais, Rui M.; Caetano, Ana P. F.; Barreiros, M. Alexandra; Abanades, Stéphane; Almeida Costa Oliveira, Fernando
- Cork-derived ceria ecoceramics for solar fuel production via thermochemical redox process using concentrated solar energyPublication . Novais, Rui M.; Oliveira, Fernando Almeida Costa; Barreiros, M. Alexandra; Abanades, Stéphane; Caetano, Ana P. F.; Pullar, Robert C.
- High performance cork-templated ceria for solar thermochemical hydrogen production via two-step water-splitting cyclesPublication . Oliveira, Fernando Almeida Costa; Barreiros, M. Alexandra; Haeussler, Anita; Caetano, Ana P. F.; Mouquinho, Ana; Silva, P. Oliveira e; Novais, Rui M.; Pullar, Robert C.; Abanades, StéphaneABSTRACT: Water splitting by solar energy-driven two-step thermochemical cycles is a promising approach for large-scale production of renewable fuels (e.g. hydrogen). The key challenge is developing materials capable of withstanding the harsh environmental conditions and to ensure high reliability in use, particularly in terms of redox kinetics and better activity at low operation temperatures. In this work, we demonstrate that cork-templated ceria can significantly enhance the hydrogen production performance under solar irradiation heating. Three types of ceria morphologies were synthesised and investigated in two-step thermochemical redox cycles, namely ceria granules (ecoceramics) prepared from cork templates based on either a green water-based or an acetone solvent-based approach, as well as ceria foams replicated from polyurethane templates. These materials were cycled in a high-temperature indirectly-irradiated solar tubular reactor, heated via concentrated solar light, using a temperature-swing process. Samples were typically thermally reduced at 1400-1450 degrees C and subsequently re-oxidised with H2O between 950-1150 degrees C. The green synthesis ceria granules had up to 25% and 32% higher average H-2 production yields than the acetone-based ecoceramics and replicated ceria foams, respectively. On average, H-2 production rates for cork-templated ceria granules (1.3 +/- 0.2 mL min(-1) g(-1)) were up to similar to 60% higher than for ceria foams (0.8 +/- 0.3 mL min(-1) g(-1)), indicating that the morphology of this three-dimensionally ordered macroporous (3-DOM) CeO2 improves the reaction kinetics. This is attributed to the smaller mean cell size of the cork-derived ecoceramic (25 mu m) compared to that of the replicated ceria foam (575 mu m), suggesting that their semi-closed wall cells enhanced reaction rates. The increase in reduction temperature from 1400 to 1450 degrees C resulted in the highest H-2 production rate (1.6 mL min(-1) g(-1)) reported so far for 3-DOM ceria. Neither loss in redox performance nor change in grain morphology was observed from the first to the last cycle. These findings show that cork-like structural features are key to engineering efficient materials for enhanced solar thermochemical fuel production.
- A review of solar thermochemical CO2 splitting using ceria-based ceramics with designed morphologies and microstructuresPublication . Pullar, Robert C.; Novais, Rui M.; Caetano, Ana P. F.; Barreiros, M. Alexandra; Abanades, Stéphane; Oliveira, Fernando Almeida CostaABSTRACT: This review explores the advances in the synthesis of ceria materials with specific morphologies or porous macro- and microstructures for the solar-driven production of carbon monoxide (CO) from carbon dioxide (CO2). As the demand for renewable energy and fuels continues to grow, there is a great deal of interest in solar thermochemical fuel production (STFP), with the use of concentrated solar light to power the splitting of carbon dioxide. This can be achieved in a two-step cycle, involving the reduction of CeO2 at high temperatures, followed by oxidation at lower temperatures with CO2, splitting it to produce CO, driven by concentrated solar radiation obtained with concentrating solar technologies (CST) to provide the high reaction temperatures of typically up to 1,500 degrees C. Since cerium oxide was first explored as a solar-driven redox material in 2006, and to specifically split CO2 in 2010, there has been an increasing interest in this material. The solar-to-fuel conversion efficiency is influenced by the material composition itself, but also by the material morphology that mostly determines the available surface area for solid/gas reactions (the material oxidation mechanism is mainly governed by surface reaction). The diffusion length and specific surface area affect, respectively, the reduction and oxidation steps. They both depend on the reactive material morphology that also substantially affects the reaction kinetics and heat and mass transport in the material. Accordingly, the main relevant options for materials shaping are summarized. We explore the effects of microstructure and porosity, and the exploitation of designed structures such as fibers, 3-DOM (three-dimensionally ordered macroporous) materials, reticulated and replicated foams, and the new area of biomimetic/biomorphous porous ceria redox materials produced from natural and sustainable templates such as wood or cork, also known as ecoceramics.
- Solar redox cycling of ceria structures based on fiber boards, foams, and biomimetic cork-derived ecoceramics for two-step thermochemical H2O and CO2 splittingPublication . Haeussler, Anita; Abanades, Stéphane; Oliveira, Fernando Almeida Costa; Barreiros, M. Alexandra; Caetano, Ana P. F.; Novais, Rui M.; Pullar, Robert C.ABSTRACT: Solar thermochemical conversion of H2O and captured CO2 is considered for the production of high-value solar fuels and CO2 valorization, using nonstoichiometric oxygen-exchange redox materials. This work aims to compare the thermochemical cycle performance of different ceria structures, including biomimetic cork-templated ceria (CTCe), ceria foams (CeF), and ceria bulk fiber boards (CeFB), to study the effect of the morphology on fuel production from two-step H2O and CO2 splitting via solar redox cycling. The considered materials underwent thermochemical cycles in a directly irradiated solar reactor under various operating conditions. Typically, a thermal reduction at 1400 degrees C under Ar at atmospheric pressure, using concentrated solar energy, was carried out followed by an oxidation step with H2O or CO2 between 800 and 1050 degrees C. The comparison of the fuel production rate and yield from the reactive materials highlighted the importance of the material thermal stability during cycling. CTCe and CeF showed good O-2 and fuel production stability over repeated cycles, while CeFB exhibited a decrease of the production because of sintering and thermal gradient due to its low thermal conductivity. Biomimetic CTCe showed a higher fuel production rate compared to the other investigated materials, explained by the favorable microstructure of the cork-based ceramic. The morphology obtained from the cork structure led to the improvement of the redox activity, demonstrating the relevance of studying this material for thermochemical H2O and CO2 splitting cycles. In addition, the impact of the operating conditions was investigated. A decrease of the starting oxidation temperature, an increase of the CO2 molar fraction (lower CO/CO2 ratio), or a high total gas flow rate favoring gas product dilution had a beneficial impact on the CO (or H-2) production rate.
- Solar thermochemical CO2 splitting using cork-templated ceria ecoceramicsPublication . Oliveira, Fernando Almeida Costa; Barreiros, M. Alexandra; Abanades, Stéphane; Caetano, Ana P. F.; Novais, Rui M.; Pullar, Robert C.ABSTRACT: This work addresses the solar-driven thermochemical production of CO and O-2 from two-step CO2-splitting cycles, using both ceria granules prepared from cork templates (CG) and ceria foams from polyurethane templates (CF). These materials were cycled in a high-temperature indirectly-irradiated solar tubular reactor using a temperature-swing process. Samples were typically reduced at 1400 degrees C using concentrated solar power as a heating source and subsequently oxidised with CO2 between 1000-1200 degrees C. On average, CO production yields for CG were two times higher than for CF, indicating that the morphology of this three-dimensionally ordered macroporous (3-DOM) CeO2 improves the reaction kinetics. Their performance stability was demonstrated by conducting 11 cycles under solar irradiation conditions. Slightly increasing the reduction temperature strongly enhanced the reduction extent, and thus the CO production yield (reaching about 0.2 mmol g(-1) after reduction at 1450 degrees C in inert gas), while decreasing the oxidation temperature mainly improved the CO production rate (up to 1.43 mu mol s(-1) g(-1) at 1000 degrees C). Characterisation of the 3-DOM structure, by means of XRD and SEM, provided insights into the reactivity behaviour of the developed materials. The pre-sintered ceria granules retained their structure after cycling. The fact that the mean cell size of CG is smaller (at least one order of magnitude) than that of CF suggests that its exposed surfaces enhanced reaction rates by a factor of two. Moreover, the maximum fuel production rate of CG was roughly three times greater than that reported previously for a ceria reticulated porous foam with dual-scale porosity.