159 results on '"Juan Antonio Cecilia"'
Search Results
2. Reversed Mg-Based Smectites: A New Approach for CO2 Adsorption
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Francisco Franco, Juan Antonio Cecilia, Laura Pardo, Salima Essih, Manuel Pozo, Lucía dos Santos-Gómez, and Rosario M. P. Colodrero
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acid treatment ,microwave ,smectites ,PCHs ,CO2 adsorption ,Chemistry ,QD1-999 - Abstract
Addressing climate change requires transitioning to cleaner energy sources and adopting advanced CO2 capture techniques. Clay minerals are effective in CO2 adsorption due to their regenerative properties. Recent advancements in nanotechnology further improve their efficiency and potential for use in carbon capture and storage. This study examines the CO2 adsorption properties of montmorillonite and saponite, which are subjected to a novel microwave-assisted acid treatment to enhance their adsorption capacity. While montmorillonite shows minimal changes, saponite undergoes significant alterations. Furthermore, the addition of silica pillars to smectites results in a new nanomaterial with a higher surface area (653 m2 g−1), denoted as reversed smectite, with enhanced CO2 adsorption capabilities, potentially useful for electrochemical devices for converting captured CO2 into value-added products.
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- 2024
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3. Adsorption of Carvone and Limonene from Caraway essential oil onto Tunisian montmorillonite clay for pharmaceutical application
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Chaima Agougui, Juan Antonio Cecilia, Houda Saad, Francisco Franco-Duro, Rym Essid, Mohamed Khabbouchi, and Najoua Frini-Srasra
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Medicine ,Science - Abstract
Abstract To explore a novel kind of green composite material having excellent antibacterial, antifungal ability and specific-targeting capability for pharmaceutical uses, a novel kind of bio-composite was prepared using sodium purified clay as carrier of Caraway essential oil (CEO). Gas chromatography-mass spectroscopy (GC–MS) analyses of CEO reveals that Carvone (68.30%) and Limonene (22.54%) are the two major components with a minimum inhibitory concentration (MIC) value equal to 125 mg/mL against Staphylococcus (S) aureus bacteria and Candida albicans fungi. Clay from Zaghouan was purified and characterized by X-ray Photoelectron Spectroscopy (XPS), X-ray diffraction (XRD), Fourier transformed infrared spectroscopy (FT-IR) and N2 adsorption–desorption (BET method). Results obtained by chromatograph equipped with a flame ionization detector (GC-FID) show that the concentration of 130 mg/mL of essential oil and 5 h of contact with the purified clay are the optimal conditions for the bio-hybrid formation. The pseudo-second-order model can describe the kinetic study of the adsorption of Carvone and Limonene on sodium montmorillonite, and the adsorption isotherms have been established to the Langmuir type. Limonene registers a maximum adsorption value equal to 3.05 mg/g of clay however Carvone register the higher amount of adsorption (19.98 mg/g) according to its polarity and the abundance of this compound in the crude CEO. X-ray diffraction, Fourier transformed infrared spectroscopy, elemental analyses (CHN) and X-ray fluorescence characterization valid the success adsorption of CEO in sodium montmorillonite surface. The purified clay/CEO hybrid (purified clay/CEO) combined the advantages of both the clay and the essential oil used in exerting the antibacterial and antifungal activity, and thus, the composite has a double antibacterial and antifungal activity compared to the separately uses of inactive clay and CEO, suggesting the great potential application in pharmaceutical treatments.
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- 2022
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4. Partial Purification of Anthocyanins (Brassica oleracea var. Rubra) from Purple Cabbage Using Natural and Modified Clays as Adsorbent
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Darlyson Tavares Guimarães, Liana Maria Ramos Mendes, Luiz Bruno de Sousa Sabino, Edy Sousa de Brito, Enrique Vilarrasa-García, Enrique Rodríguez-Castellón, Juan Antonio Cecilia, and Ivanildo José da Silva Junior
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Physical and theoretical chemistry ,QD450-801 - Abstract
This research is aimed at evaluating strategies for the adsorption and recovery of anthocyanins present in purple cabbage using natural and modified clays as adsorbent. In the batch adsorption experiments, the anthocyanin extracts were put in contact with the adsorbents, and different parameters were evaluated to determine the best conditions for their adsorption and recovery. It was noted that the highest levels of adsorption (28.0 mg g-1) occurred using a porous clay heterostructure (PCH) material as adsorbent, with a mass of 25 mg and 120 min of contact. Under the same conditions, the sepiolite only presented an adsorption capacity of 14.0 mg g-1. The desorption results showed that the 60% methanolic solution recovered 60% of the anthocyanins adsorbed on PCH, while the 80% ethanolic solution recovered 35% of those adsorbed on sepiolite. The eluted anthocyanin solutions showed a 98% lower sugar concentration than the crude extract, indicating the low affinity of the adsorbents for sugars. Six types of acylated cyanidins were identified via UPLC-QToF-MSE in the extract, and it was confirmed from the FTIR analyses that the highest affinity of the clays occurred with the anthocyanins that presented more organic acid in their structure. The results show that PCH and sepiolite have high selectivity for anthocyanins and low affinity for the sugars present in the plant extract, facilitating the process of partial purification and application of these pigments.
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- 2023
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5. Assessing CO2 Adsorption on Amino-Functionalized Mesocellular Foams Synthesized at Different Aging Temperatures
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Enrique Vilarrasa-García, Juan Antonio Cecilia, Pedro Augusto S. Moura, Diana C. S. Azevedo, and Enrique Rodríguez-Castellón
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silica ,mesocellular foam ,synthesis ,amino groups ,CO2 adsorption ,Chemistry ,QD1-999 - Abstract
A wide variety of solid sorbents has recently been synthesized for application in CO2 adsorption. Among them, mesoporous silicas deserve attention because of their ability to accommodate large concentrations of different chemicals as a consequence of their surface chemistry and tunable pore structure. Functionalized materials exhibit promising features for CO2 adsorption at high temperatures and low CO2 concentrations. This work aimed to assess the influence of the textural properties on the performance of CO2 adsorption on functionalized mesoporous silica. With this goal, several mesoporous silica foams were synthesized by varying the aging temperature, obtaining materials with larger pore diameter. Thus, the synthesized materials were functionalized by grafting or impregnation with 3-aminopropyltriethoxysilane, polyethylenimine, and tetraethylenepentamine as amine sources. Finally, the amino functionalized materials were assessed for CO2 capture by means of equilibrium adsorption isotherms at 25, 45, and 65°C. Among the most outstanding results, high aging temperatures favor the performance of impregnated materials by exposing greater pore diameters. Low or intermediate temperatures favor grafting by preserving an appropriate density of silanol groups.
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- 2020
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6. CO2 Capture by Reduced Graphene Oxide Monoliths with Incorporated CeO2 Grafted with Functionalized Polymer Brushes
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Nikolaos Politakos, Luis Serrano Cantador, Juan Antonio Cecilia, Iranzu Barbarin, and Radmila Tomovska
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reduced graphene oxide ,monolith ,polymer brushes ,cerium oxide ,RAFT polymerization ,CO2 adsorption ,Technology ,Engineering (General). Civil engineering (General) ,TA1-2040 ,Biology (General) ,QH301-705.5 ,Physics ,QC1-999 ,Chemistry ,QD1-999 - Abstract
The monolithic materials of reduced graphene oxide (rGO) can be used successfully in CO2 adsorption. Here, the incorporation of CeO2 particles with and without polymer brushes grafted from the particles showed that the structural properties could be changed, affecting the adsorption of CO2. Polymer brushes of (1) poly(acrylic acid) (PAA), (2) poly(vinyl caprolactam) (PVCL) and (3) poly[(2-(methacryloyloxy)ethyl) trimethylammonium chloride] (PMETAC) were grafted from CeO2 via reversible addition−fragmentation chain transfer (RAFT) polymerization. The preparation of monoliths of rGO with different modified CeO2 particles led to different thermal properties (TGA), structural changes (BET isotherms) and CO2 adsorption. The responsive character of the CeO2@polymer was proven by the DLS and UV results. The responsive character of the particles incorporated into the rGO monolith affected not only the adsorption capacity but also the microstructure and values of the surface volume of the pores of the monolith. Monoliths with porosity values for better adsorption were affected by the responsive character of the polymer.
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- 2021
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7. Effect of Polyvinyl Alcohol Ligands on Supported Gold Nano-Catalysts: Morphological and Kinetics Studies
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Stefano Scurti, Eleonora Monti, Elena Rodríguez-Aguado, Daniele Caretti, Juan Antonio Cecilia, and Nikolaos Dimitratos
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gold nanoparticles ,hydrogenation of 4-nitrophenol ,polyvinyl alcohol ligands ,Chemistry ,QD1-999 - Abstract
The effect of polyvinyl alcohol (PVA) stabilizers and gold nanoparticles supported on active carbon (AuNPs/AC) was investigated in this article. Polymers with different molecular weights and hydrolysis degrees have been synthesized and used, like the stabilizing agent of Au nano-catalysts obtained by the sol-immobilization method. The reduction of 4-nitrophenol with NaBH4 has been used as a model reaction to investigate the catalytic activity of synthesized Au/AC catalysts. In addition, we report several characterization techniques such as ultraviolet-visible spectroscopy (UV-Vis), dynamic light scattering (DLS), X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) in order to correlate the properties of the polymer with the metal nanoparticle size and the catalytic activity. A volcano plot was observed linking the catalytic performance with hydrolysis degree and the maximum of the curve was identified at a value of 60%. The Au:PVA-60 weight ratio was changed in order to explain how the amount of the polymer can influence catalytic properties. The effect of nitroaromatic ring substituents on the catalytic mechanism was examined by the Hammett theory. Moreover, the reusability of the catalyst was investigated, with little to no decrease in activity observed over five catalytic cycles. Morphological and kinetic studies reported in this paper reveal the effect of the PVA polymeric stabilizer properties on the size and catalytic activity of supported gold nanoparticles.
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- 2021
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8. CO2 Valorization and Its Subsequent Valorization
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Juan Antonio Cecilia, Daniel Ballesteros Plata, and Enrique Vilarrasa García
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n/a ,Organic chemistry ,QD241-441 - Abstract
After the industrial revolution, the increase in the world population and the consumption of fossil fuels has led to an increase in anthropogenic CO2 emissions [...]
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- 2021
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9. Chitosan: A Natural Biopolymer with a Wide and Varied Range of Applications
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Carmen P. Jiménez-Gómez and Juan Antonio Cecilia
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chitin ,chitosan ,biomaterial ,adsorbent ,antioxidant ,high added value product ,Organic chemistry ,QD241-441 - Abstract
Although chitin is of the most available biopolymers on Earth its uses and applications are limited due to its low solubility. The deacetylation of chitin leads to chitosan. This biopolymer, composed of randomly distributed β-(1-4)-linked D-units, has better physicochemical properties due to the facts that it is possible to dissolve this biopolymer under acidic conditions, it can adopt several conformations or structures and it can be functionalized with a wide range of functional groups to modulate its superficial composition to a specific application. Chitosan is considered a highly biocompatible biopolymer due to its biodegradability, bioadhesivity and bioactivity in such a way this biopolymer displays a wide range of applications. Thus, chitosan is a promising biopolymer for numerous applications in the biomedical field (skin, bone, tissue engineering, artificial kidneys, nerves, livers, wound healing). This biopolymer is also employed to trap both organic compounds and dyes or for the selective separation of binary mixtures. In addition, chitosan can also be used as catalyst or can be used as starting molecule to obtain high added value products. Considering these premises, this review is focused on the structure and modification of chitosan as well as its uses and applications.
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- 2020
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10. Relevance of the Physicochemical Properties of Calcined Quail Eggshell (CaO) as a Catalyst for Biodiesel Production
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Leandro Marques Correia, Juan Antonio Cecilia, Enrique Rodríguez-Castellón, Célio Loureiro Cavalcante, and Rodrigo Silveira Vieira
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Chemistry ,QD1-999 - Abstract
The CaO solid derived from natural quail eggshell was calcined and employed as catalyst to produce biodiesel via transesterification of sunflower oil. The natural quail eggshell was calcined at 900°C for 3 h, in order to modify the calcium carbonate present in its structure in CaO, the activity phase of the catalyst. Both precursor and catalyst were characterized using Hammett indicators method, X-ray fluorescence (XRF), X-ray diffraction (XRD), thermogravimetric analysis (TG/DTG), CO2 temperature-programmed desorption (CO2-TPD), X-ray photoelectronic spectroscopy (XPS), Fourier infrared spectroscopy (FTIR), scanning electron microscopy (SEM), N2 adsorption-desorption at −196°C, and distribution particle size. The maximum biodiesel production was of 99.00 ± 0.02 wt.% obtained in the following transesterification reaction conditions: XMR (sunflower oil/methanol molar ratio of 1 : 10.5 mol : mol), XCAT (catalyst loading of 2 wt.%), XTIME (reaction time of 2 h), stirring rate of 1000 rpm, and temperature of 60°C.
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- 2017
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11. Separation of Light Liquid Paraffin C5–C9 with Cuban Volcanic Glass Previously Used in Copper Elimination from Water Solutions
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Miguel Autie-Pérez, Antonia Infantes-Molina, Juan Antonio Cecilia, Juan M. Labadie-Suárez, and Enrique Rodríguez-Castellón
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glass ,adsorption ,surface properties ,copper removal ,IGC ,paraffins ,Technology ,Engineering (General). Civil engineering (General) ,TA1-2040 ,Biology (General) ,QH301-705.5 ,Physics ,QC1-999 ,Chemistry ,QD1-999 - Abstract
Featured Application: In this work, an inexpensive and available material, as volcanic glass, is used to absorb metals from wastewater and then it is used to the separation of light liquid-olefins.Abstract: Raw porous volcanic glass from Cuba was used as an adsorbent for Cu2+ removal from dyes after activation with an acid solution. After Cu2+ adsorption, it was also evaluated its capacity to separate n-paraffins from a mixture by inverse gas chromatography (IGC), and the results were compared with those obtained with bare volcanic glass without copper. The main goal of this work is to highlight the great applicability of natural volcanic glass, which can be reused without pretreatment as an adsorbent. The results from copper adsorption were quite promising, considering the availability and low cost of this material; the sample without acid treatment turned out to be the most adequate to remove copper. Moreover, the results from IGC revealed that the separation of paraffins from the mixture was achieved with both bare volcanic glass and glass containing Cu, although greater heat adsorption values were obtained when copper was present in the sample due to the stronger interaction between paraffin and copper. The high availability and low cost of this porous material make it a potential and attractive candidate to be used in both heavy metal removal and paraffin separation for industrial purposes.
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- 2018
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12. Influence of Lewis and Brønsted acid catalysts in the transformation of hexoses into 5-ethoxymethylfurfural
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Benjamín Torres-Olea, Inmaculada Fúnez-Núñez, Cristina García-Sancho, Juan Antonio Cecilia, Ramón Moreno-Tost, and Pedro Maireles-Torres
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Renewable Energy, Sustainability and the Environment - Published
- 2023
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13. Influence of stabilisers on the catalytic activity of supported Au colloidal nanoparticles for the liquid phase oxidation of glucose to glucaric acid: understanding the catalyst performance from NMR relaxation and computational studies
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Eleonora Monti, Alessia Ventimiglia, Luke Forster, Elena Rodríguez-Aguado, Juan Antonio Cecilia, Francesca Ospitali, Tommaso Tabanelli, Stefania Albonetti, Fabrizio Cavani, Ivan Rivalta, Carmine D'Agostino, and Nikolaos Dimitratos
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Environmental Chemistry ,Pollution - Abstract
Impact of stabilisers on the catalytic performance of supported Au colloidal nanoparticles for the liquid phase oxidation of glucose to glucaric acid.
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- 2023
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14. Tailoring of Textural Properties of 3D Reduced Graphene Oxide Composite Monoliths by Using Highly Crosslinked Polymer Particles toward Improved CO2 Sorption
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Iranzu Barbarin, Nikolaos Politakos, Luis Serrano Cantador, Juan Antonio Cecilia, Oihane Sanz, and Radmila Tomosvka
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Polymers and Plastics ,polymer composites ,Process Chemistry and Technology ,Organic Chemistry ,mesoporosity ,microporosity ,reduced graphene oxide ,CO2 capture ,3D porous monoliths - Abstract
The main constraint on developing a full potential for CO2 adsorption of 3D composite monoliths made of reduced graphene oxide (rGO) and polymer materials is the lack of control of their textural properties, along with the diffusional limitation to the CO2 adsorption due to the pronounced polymers' microporosity. In this work, the textural properties of the composites were altered by employing highly crosslinked polymer particles, synthesized by emulsion polymerization in aqueous media. For that aim, waterborne methyl methacrylate (MMA) particles were prepared, in which the crosslinking was induced by using different quantities of divinyl benzene (DVB). Afterward, these particles were combined with rGO platelets and subjected to the reduction-induced self assembly process. The resulting 3D monolithic porous materials certainly presented improved textural properties, in which the porosity and BET surface area were increased up to 100% with respect to noncrosslinked composites. The crosslinked density of MMA polymer particles was a key parameter controlling the porous properties of the composites. Consequently, higher CO2 uptake than that of neat GO structures and composites made of noncrosslinked MMA polymer particles was attained. This work demonstrates that a proper control of the microstructure of the polymer particles and their facile introduction within rGO self assembly 3D structures is a powerful tool to tailor the textural properties of the composites toward improved CO2 capture performance. I.B. gratefully acknowledges the financial support of the Spanish Government (BES-2017-080221). L.S. thank s the grant P20_00328 funded by the Consejeria de Transformacion Economica, Industria, Conocimiento y Universidades of the Junta de Andalucia and by the EU FEDER funds. The authors thank the technical and human support provided by SGIker (UPV/EHU/ERDF, EU).
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- 2022
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15. Increased Protonation of a Mesopore Surface in a Porous Clay Nanoheterostructure
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Kiminori Sato, Eikichi Fujikawa, and Juan Antonio Cecilia
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General Energy ,Physical and Theoretical Chemistry ,Surfaces, Coatings and Films ,Electronic, Optical and Magnetic Materials - Published
- 2022
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16. Effect of Capping Ligands for the Synthesis of Gold Nanoparticles and on the Catalytic Performance for the Oxidation of 5-Hydroxymethyl-2-furfural
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Albonetti, Francesca Liuzzi, Alessia Ventimiglia, Alessandro Allegri, Elena Rodríguez-Aguado, Juan Antonio Cecilia, Ivan Rivalta, Nikolaos Dimitratos, and Stefania
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gold nanoparticles ,stabilizer effect ,polymers ,HMF oxidation ,sol-immobilization ,DFT ,cluster - Abstract
Different series of Au on carbon catalysts were prepared via sol-immobilization to investigate the role of polymers (polyvinylpyrrolidone PVP, polyethylene glycol PEG and polyvinyl alcohol PVA), employed as gold nanoparticle (NP) stabilizers, on catalyst properties and on catalytic activity. The synthesized materials were widely characterized with several techniques (DLS, XRD, TEM and XPS) and used as catalysts in the 5-hydroxymethylfurfural (HMF) oxidation to produce 2,5-furandicarboxylic acid (FDCA). The obtained results clearly demonstrated the PVA leading to the formation of smaller and more active NPs. On the contrary, polyethylene glycol was shown to affect gold exposure and, as a consequence, to reduce the catalyst activity due to steric effects while PVP-based catalysts presented bigger and more covered Au NPs. The investigation on the reusability of the catalysts demonstrated the presence of a significant deactivation on all prepared materials, but the presence of higher amounts of polymer seems to have a positive effect on catalyst stability even if associated with lower reactivity. Computational studies have provided interesting information on the NP-polymer interactions and consequently on the catalytic activities.
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- 2023
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17. Applicability of mesoporous silica type SBA-15 as feasible support for the immobilization of Yarrowia lipolytica lipase and Candida antarctica lipase B
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Nathália Saraiva Rios, Talita Lopes Honorato, Juan Antonio Cecilia, Enrique Rodríguez-Castellón, Maria Alice Zarur Coelho, Ivanildo José da Silva Júnior, and Luciana Rocha Barros Gonçalves
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General Chemical Engineering - Published
- 2022
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18. Highly dispersed copper oxide on silica: Towards an efficient catalyst for continuous glycerol dehydration to acetol
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Jaime Mazarío, Juan Antonio Cecilia, Enrique Rodriguez Castellon, Marcelo E. Domine, and Ministerio de Economía y Competitividad (España)
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History ,Polymers and Plastics ,Process Chemistry and Technology ,Business and International Management ,Industrial and Manufacturing Engineering ,Catalysis - Abstract
In most current processes aimed at producing biodiesel glycerol is still a co-product, and its valorisation is essential for the biorefinery. This work relies on previous results showing the dependence of the selective dehydration of glycerol to acetol (hydroxyacetone) on achieving a moderate acidity and the redox functionality of copper to complete the chemical process. In this sense, this reaction was studied using CuO supported on silica. Different silicas and copper incorporation methodologies were investigated to develop the best CuO/SiO material. Interestingly, these CuO-based materials developed acidity and became more active when increasing the copper oxide dispersion, thereby going from poorly to intensely effective to dehydrate glycerol selectively to acetol. Catalysts were characterised by different techniques (i.e., ICP, N adsorption, XRD, TPR, HR-TEM, etc.) to explain the differences observed in catalytic activity and acetol yield based on their physicochemical properties., Financial support by Spanish Government (CTQ-2015-67592, PGC2018-097277-B-I00 and SEV-2016-0683) is gratefully acknowledged. J.M. thanks Spanish Government (CTQ-2015-67592) for the Ph.D. fellowship. Authors also thank Miriam Parreño Romero and the Electron Microscopy Service of Universitat Politècnica de València for their support.
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- 2023
19. Glyphosate adsorption onto porous clay heterostructure (PCH): kinetic and thermodynamic studies
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Enrique Vilarrasa-García, Juan Antonio Cecilia, Enrique Rodríguez-Castellón, Nesrine Chouikhi, Mohamed Bagane, Mohamed Chlendi, and Sabrine Besghaier
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Glyphosate ,Langmuir ,Chemistry ,General Chemical Engineering ,Inorganic chemistry ,PCH ,Sorption ,Endothermic process ,Silanol ,chemistry.chemical_compound ,Adsorption ,Montmorillonite ,Organophosphate ,Glifosato ,Bentonite ,Porous clay heterostructures - Abstract
The synthesis of PCH from natural bentonite produces a porous heterostructure material effective for the adsorption of glyphosate from water. The adsorption process takes place through an interaction between the silanol group of montmorillonite and/or the PCH adsorbent with the functional groups of glyphosate. The glyphosate adsorption isotherms, recorded for all the studied samples, have been established to be of Langmuir type. The kinetic of the herbicide adsorption on the PCH was best described by the pseudo-second-order model. With the increase in temperature from 25 to 50 °C, the sorption capacities of the materials studied towards glyphosate increased. The process of glyphosate adsorption was found to be endothermic and spontaneous in nature, as indicated by positive values of ΔH and negative values of ΔG. According to the results obtained, the herbicide sorption was more effective in a basic environment. The maximum amount of adsorbed glyphosate is almost doubled with PCH from 13.5 mg/g of natural clay to 27.5 mg/g of PCH. This study was partially funded by project RTI2018-099668-BC22 of Ministerio de Ciencia, Innovación y Universidades, and project UMA18-FEDERJA-126 of Junta de Andalucía and FEDER funds. Open Access funding provided thanks to the CRUE-CSIC agreement with Springer Nature and Funding for open access charge: Universidad de Málaga / CBUA.
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- 2021
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20. Mixed Oxides Derived from Hydrotalcites Mg/Al Active in the Catalytic Transfer Hydrogenation of Furfural to Furfuryl Alcohol
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Raquel López-Asensio, Juan Antonio Cecilia-Buenestado, Concepción Herrera-Delgado, María Ángeles Larrubia-Vargas, Cristina García-Sancho, Pedro Jesús Maireles-Torres, and Ramón Moreno-Tost
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hydrotalcite ,MPV reaction ,furfural ,isopropanol ,FTIR spectroscopy ,Physical and Theoretical Chemistry ,Catalysis ,General Environmental Science - Abstract
Herein, a family of Mg/Al hydrotalcites was synthesized as catalytic precursors of MgAlOx mixed oxides. Both hydrotalcites and mixed oxides were characterized and the mixed oxides were tested in the reduction of furfural to yield furfuryl alcohol by MPV reaction using isopropanol as hydrogen donor. Different catalytic parameters were tested, such as the type of alcohol, calcination temperature of the hydrotalcite, and reaction temperature. Furfural and isopropanol were adsorbed on the MgAl-3 catalyst to follow the species adsorbed on the catalyst by FTIR analysis. The results showed that the isopropanol was activated as isopropoxide and furfural changed the adsorption site with increasing temperature but maintaining the h1-conformation. The catalytic performances were associated with the basicity of the catalysts and the deactivation processes have been attributed to the existence of adsorbed species on the surface, mainly due to furfural-derived compounds. The catalysts were reused in three consecutive cycles showing a sharp drop of catalytic activity. To recover the activity, the catalysts were calcined at 500 °C but the activity was only partially recovered. The XPS analysis after reactivation showed that the catalyst surface was modified due to the segregation of hydroxides of Mg and Al.
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- 2022
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21. Recent Advances in Mesoporous Materials and Their Biomedical Applications
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Ramon Moreno-Tost and Juan Antonio Cecilia
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Inorganic Chemistry ,Organic Chemistry ,Biocompatible Materials ,General Medicine ,Physical and Theoretical Chemistry ,Molecular Biology ,Porosity ,Spectroscopy ,Catalysis ,Computer Science Applications - Abstract
Since the beginning of civilization, porous materials have been used for medical purposes [...]
- Published
- 2022
22. Modification of the Textural Properties of Chitosan to Obtain Biochars for CO
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Isabel, Barroso-Martín, Juan Antonio, Cecilia, Enrique, Vilarrasa-García, Daniel, Ballesteros-Plata, Carmen Pilar, Jiménez-Gómez, Álvaro, Vílchez-Cózar, Antonia, Infantes-Molina, and Enrique, Rodríguez-Castellón
- Abstract
Three chitosans with different morphologies have been used (commercial chitosan powder, chitosan in film form and chitosan in globular form synthesized by the freeze-dried method) for the synthesis of biochars. The pyrolytic treatment has revealed that the biochar synthesized from the chitosan formed by the freeze-dried method reaches the highest CO
- Published
- 2022
23. PdO Supported on TiO2 for the Oxidative Condensation of Furfural with Ethanol: Insights on Reactivity and Product Selectivity
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Juan Antonio Cecilia, Pedro Maireles-Torres, Cristina García-Sancho, Virginia Torres-Bujalance, Ramón Moreno-Tost, Lerato F.E. Machogo, Rafael Luque, and Carmen P. Jiménez-Gómez
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Ethanol ,Renewable Energy, Sustainability and the Environment ,General Chemical Engineering ,Condensation ,General Chemistry ,Oxidative phosphorylation ,Furfural ,chemistry.chemical_compound ,chemistry ,Product (mathematics) ,Environmental Chemistry ,Organic chemistry ,Reactivity (chemistry) ,Selectivity - Published
- 2021
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24. H2S and H2O Combined Effect on CO2 Capture by Amino Functionalized Hollow Microsphere Silicas
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Moises Bastos-Neto, J. L. B. de Oliveira, Rafael Morales-Ospino, Enrique Rodríguez-Castellón, J. A. R. de Sousa, Juan Antonio Cecilia, R. Amâncio, Diana C. S. Azevedo, and Enrique Vilarrasa-García
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Materials science ,Chemical engineering ,General Chemical Engineering ,General Chemistry ,Industrial and Manufacturing Engineering ,Amino functionalized ,Microsphere - Published
- 2021
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25. Conversion of Lignocellulosic Biomass to Biofuels
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Cristina García-Sancho, Juan Antonio Cecilia, and Rafael Luque
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Chemistry ,Biofuel ,Lignocellulosic biomass ,Ethyl levulinate ,Pulp and paper industry - Published
- 2021
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26. Comparative Electrochemical Study of Pure Magnesium Behavior in Ringer’s and Hank’s Solutions
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Enrique Rodríguez-Castellón, Juan Antonio Cecilia-Buenestado, Samia Ben Hassen, Yasser Ben Amor, and Marwa Hattab
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Materials science ,Scanning electron microscope ,Brucite ,Magnesium ,020209 energy ,Organic Chemistry ,Metals and Alloys ,chemistry.chemical_element ,02 engineering and technology ,engineering.material ,021001 nanoscience & nanotechnology ,Microstructure ,Surfaces, Coatings and Films ,Corrosion ,Dielectric spectroscopy ,Chemical engineering ,chemistry ,X-ray photoelectron spectroscopy ,0202 electrical engineering, electronic engineering, information engineering ,Materials Chemistry ,engineering ,0210 nano-technology ,Dissolution - Abstract
A corrosion study of high purity magnesium in two simulated physiological solutions (Ringer’s solution and Hank’s solution) is reported. The electrochemical behavior of pure magnesium rotating disc electrode (RDE) was examined using electrochemical impedance spectroscopy (EIS) and potentiodynamic polarization (PDP) techniques. The rotation affects the potentiodynamic polarisation curves and makes a shift in the anodic branches because of the dissolution of the corrosion layer. The EIS results showed the presence of three-time constant attributed to formation of the protective film on the Mg surface, the faradic process and the adsorption phenomena. The formation of a compact layer on magnesium surface, offers a higher corrosion protective ability for Mg. The thickness of this layer increase subsequently with increase in immersion time. The magnesium surface morphology was characterized by scanning electron microscopy (SEM). The composition and the microstructure of the corrosion product film were carried out using X-ray photoelectric spectroscopy (XPS) and X-ray diffraction (XRD). Brucite, calcite and magnesium calcite were detected in both medium, while aggregated particles containing a high concentration of phosphorus were formed on Mg in Hunk’s solution.
- Published
- 2021
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27. Production of biolubricants from soybean oil: Studies for an integrated process with the current biodiesel industry
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Ítalo C. Rios, João Paulo C. Marques, Expedito J. S. Parente, Juan Antonio Cecilia, Francisco Murilo Tavares de Luna, Enrique Rodríguez-Castellón, and Célio L. Cavalcante
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Biodiesel ,Materials science ,food.ingredient ,010405 organic chemistry ,General Chemical Engineering ,02 engineering and technology ,General Chemistry ,Transesterification ,021001 nanoscience & nanotechnology ,Oleochemical ,Pulp and paper industry ,01 natural sciences ,Soybean oil ,0104 chemical sciences ,chemistry.chemical_compound ,food ,chemistry ,Scientific method ,Viscosity index ,0210 nano-technology - Abstract
The competitiveness of the biodiesel industry may be improved by adding value through co-products and integration with the oleochemical industry, especially for novel products such as biolubricants, a product of increasing world demand. In this study the synthesis of biolubricants from soybean oil was evaluated using transesterification, epoxidation and oxirane ring opening reactions. Water, 2-ethylhexanol and their mixtures were used to obtain hydroxyl-rich and/or ether-type branched molecules. All chemical modifications were monitored by Nuclear Magnetic Resonance (1H NMR) and evaluated through the physicochemical properties of the products. Several potential biolubricant samples were synthesized with viscosities at 40 °C ranging from 26.6 to 99.6 cSt, viscosity index from 26 to 139, densities at 20 °C from 0.925 to 0.964 g/cm3, and pour points from −3 to −12 °C. From these results, a proposal of a feasible industrial process for the production of biolubricants from soybean oil is presented, consisting of 16 units, of which 15 may be integrated with an existing biodiesel plant.
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- 2021
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28. The relevance of Lewis acid sites on the gas phase reaction of levulinic acid into ethyl valerate using CoSBA-xAl bifunctional catalysts
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Pedro Maireles-Torres, James A. Dumesic, Juan Antonio Cecilia, Carmen P. Jiménez-Gómez, M. Muñoz-Olasagasti, M. López Granados, and Rafael Mariscal
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chemistry.chemical_classification ,010405 organic chemistry ,chemistry.chemical_element ,010402 general chemistry ,01 natural sciences ,Medicinal chemistry ,Catalysis ,0104 chemical sciences ,Solvent ,chemistry.chemical_compound ,Acid strength ,chemistry ,Yield (chemistry) ,Levulinic acid ,Lewis acids and bases ,Bifunctional ,Cobalt - Abstract
A series of Co supported on Al-modified SBA-15 catalysts has been studied in the gas phase direct transformation of levulinic acid (LA) into ethyl valerate (EV) using a continuous fixed-bed reactor and ethanol as solvent. It was observed that once the intermediate product gamma-valerolactone (GVL) has been formed, the presence of aluminum is required for the selective transformation to EV. Three Lewis acid sites (LAS) are identified (from highest to lowest acid strength): aluminum ions in tetrahedral and octahedral coordination and Co2+ sites. The intrinsic activity of these LAS for the key reaction, the GVL ring opening, decreases with the strength of these acid sites, but so does the undesirable formation of coke, also catalyzed by these centers. The best catalyst was that with the highest Al content, CoSBA-2.5Al, that reached an EV yield of up to 70%. This result is associated with the presence of LAS attributed to the presence of Co2+ surface species that, although having low intrinsic activity in the selective GVL ring-opening reaction, are highly concentrated in this sample and also possess less activity in the undesirable and deactivating formation of coke. These Co2+ LAS have been stabilized by incorporation of aluminum into the support, modifying the reducibility and dispersion of cobalt species. Additionally, the lower proportion of metallic Co species decreases the hydrogenating capacity of this catalyst. This decrease is a positive result because it prevents GVL hydrogenation to undesired products. This catalyst also showed promising stability in a 140 h on-stream run.
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- 2021
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29. Glycerol etherification towards selective diglycerol over mixed oxides derived from hydrotalcites: effect of Ni loading
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Ramón Moreno-Tost, Enrique Rodríguez-Castellón, Juan Antonio Cecilia, M. Aloui, M. Said Zina, and Salwa Bougacha Ghorbel
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Thermogravimetric analysis ,Materials science ,Hydrotalcite ,Coprecipitation ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Condensed Matter Physics ,01 natural sciences ,0104 chemical sciences ,Electronic, Optical and Magnetic Materials ,Catalysis ,law.invention ,Biomaterials ,law ,Desorption ,Materials Chemistry ,Ceramics and Composites ,Calcination ,0210 nano-technology ,Selectivity ,Isomerization ,Nuclear chemistry - Abstract
A series of tetrametallic hydrotalcite with different Ni loading, were synthesized by coprecipitation method. Then, these hydrotalcites were calcined in their respective metal oxides and were used as catalysts in the etherification reaction for the synthesis of polyglycerols. The effect of Ni loading on the structural and textural features was investigated by various techniques such as X-ray diffraction (XRD), thermogravimetric analysis TG–DSC–MS, temperature-programmed reduction (H2-TPR), temperature-programmed desorption (NH3-TPD) and 1-butene isomerization as a model reaction to probe acid–base character of catalysts. Mixed oxides derived from hydrotalcites are found to be active and suitable, via solvent free, in the glycerol etherification reaction. A gradual enhance of glycerol conversion is revealed when increasing the Ni/Mg molar ratio and the most active catalyst found is HTc-Ni75% with full selectivity to diglycerol.
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- 2020
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30. Recovery of pentoses-containing olive stones for their conversion into furfural in the presence of solid acid catalysts
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I. Fúnez-Núñez, Juan Antonio Cecilia, Cristina García-Sancho, Pedro Maireles-Torres, L. Serrano-Cantador, and Ramón Moreno-Tost
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Olive stones ,Environmental Engineering ,Solid acid catalysts ,General Chemical Engineering ,0211 other engineering and technologies ,Fraction (chemistry) ,Pentosas ,02 engineering and technology ,010501 environmental sciences ,Xylose ,Raw material ,Furfural ,01 natural sciences ,Catalysis ,chemistry.chemical_compound ,Hydrolysis ,medicine ,Environmental Chemistry ,Xylose dehydration ,Dehydration ,Catálisis ,Safety, Risk, Reliability and Quality ,0105 earth and related environmental sciences ,021110 strategic, defence & security studies ,Chemistry ,medicine.disease ,Lignocellulosic biomass ,Yield (chemistry) ,Hemicellulosic liquors ,Nuclear chemistry - Abstract
Olive stones were employed as feedstock for furfural production in two stages: 1) autohydrolysis of hemicellulosic fraction to recover their pentoses, mainly xylose, and 2) subsequent dehydration of pentoses into furfural. Autohydrolysis step was optimized by using different experimental conditions (temperature: 160-200 ºC and time: 30-75 min), giving rise to liquors with different xylose concentrations, since hydrolysis was incomplete in some cases. The combined use of a commercial γ-Al2O3 and CaCl2 led to total hydrolysis of non-hydrolyzed pentosans after autohydrolysis step, and the subsequent dehydration of pentoses into furfural. The maximum values of furfural yield and efficiency were 23 and 96%, respectively, after only 60 minutes at 150 ºC by using liquor obtained by autohydrolysis at 180 ºC and 30 min (L5.1) as source of pentoses. This liquor, L5.1, provided better catalytic results than other liquors which had shown higher xylose concentration after autohydrolysis, probably due to these latter also exhibited a higher concentration of organic acids; thus, the presence of organic acids such as acetic and lactic acid could promote side undesired reactions leading to lower furfural yields. Finally, γ-Al2O3 was more effective for furfural production under these experimental conditions than other solid acid catalysts, such as mesoporous Nb2O5, Nb-doped SBA-15 and Zr-doped HMS silicas, probably due to alumina has a higher density of acid sites. Spanish Ministry of Economy and Competitiveness (RTI2018-94918-B-C44 project), Junta de Andalucía (RNM-1565), FEDER (European Union) funds (UMA18-FEDERJA-171) and Malaga University. C.G.S. and J.A.C. thank to FEDER funds and Malaga University respectively for financial support. L.S.C. gratefully acknowledges support from Spanish MINECO via the concession of a Ramon y Cajal contract (RYC-2015-17109).
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- 2020
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31. Graphene-Based Monolithic Nanostructures for CO2 Capture
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Radmila Tomovska, Iranzu Barbarin, Luis Serrano Cantador, Ehsan Mehravar, Nikolaos Politakos, and Juan Antonio Cecilia
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Pressure drop ,Mass transport ,Nanostructure ,Materials science ,Graphene ,General Chemical Engineering ,Nanotechnology ,02 engineering and technology ,General Chemistry ,021001 nanoscience & nanotechnology ,Industrial and Manufacturing Engineering ,law.invention ,020401 chemical engineering ,law ,0204 chemical engineering ,0210 nano-technology - Abstract
Monolithic nanocarbon-based CO2 solid sorbents offer fast mass transport, easy handling, minor pressure drop and cycle operation stability due to the interconnected three-dimensional network of por...
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- 2020
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32. Photocatalyzed preferential oxidation of CO under simulated sunlight using Au–transition metal oxide–sepiolite catalysts
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Loretta Storaro, Juan Antonio Cecilia, Antonia Infantes-Molina, Aldo Talon, Elena Rodríguez Aguado, Enrique Rodríguez-Castellón, and Elisa Moretti
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Materials science ,Oxide ,Nanoparticle ,simulated sunlight ,02 engineering and technology ,010402 general chemistry ,01 natural sciences ,transition metals ,Catalysis ,Inorganic Chemistry ,Metal ,chemistry.chemical_compound ,Photo CO oxidation ,sepiolite ,photocatalysis ,Transition metal ,Settore CHIM/03 - Chimica Generale e Inorganica ,Sepiolite ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,Chemical engineering ,chemistry ,visual_art ,Photocatalysis ,visual_art.visual_art_medium ,0210 nano-technology ,BET theory - Abstract
In the present study a series of Au–transition metal oxides supported on a clay mineral such as sepiolite were tested in the preferential oxidation of CO in an excess of H2 under simulated solar light irradiation and in the absence of light, at 30 °C and atmospheric pressure. Transition metal oxides (ZnO, Fe2O3, NiO, MnO2, and Co3O4) were dispersed over the sepiolite surface where, subsequently, Au nanoparticles with an average particle size between 2 and 3 nm were successfully deposited–precipitated. The obtained photocatalysts were characterized by XRD, XRF, DRUV-Vis, N2 adsorption–desorption and HRTEM in order to evaluate the optical, structural and chemical properties of the prepared samples. Despite the low amount of gold (nominal 1.0 wt%), the catalysts exhibited an outstanding behavior under light irradiation, with reaction rates between 4.5 and 5.2 mmol COox gcat−1 h−1 for the Au–NiSep, Au–CoSep and Au–ZnSep samples. These photocatalysts exhibited a high dispersion of the respective transition metal oxides over the sepiolite support and the presence of low-coordinated hemispherical gold nanoparticles. The superior photocatalytic efficiency of these samples was ascribed to the reduction of the electron–hole pair recombination of photogenerated charge carriers by the excitation of the localized surface plasmon resonance of the Au nanoparticles. The BET surface area and the gold particle size seemed to be relevant factors affecting the catalytic performance.
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- 2020
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33. Insights into optimized synthesis conditions of hollow microspheres of silica for water vapor adsorption
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Moises Bastos-Neto, Diana C. S. Azevedo, Enrique Rodríguez-Castellón, Juan Antonio Cecilia, Bianca Ferreira dos Santos, and Enrique Vilarrasa-García
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Silica-Based materials ,Morphology (linguistics) ,Materials science ,Scanning electron microscope ,General Chemical Engineering ,General Chemistry ,Natural gas ,Synthesis ,Adsorption ,Volume (thermodynamics) ,Chemical engineering ,Transmission electron microscopy ,Specific surface area ,Water harvesting ,Porosity ,Water vapor ,Drying - Abstract
Hollow microspheres of silica were synthesized with different ethanol/water ratios (0.4, 1.0, 2.0 and 6.0) to assess the influence of this parameter on the morphology/porosity of the samples and thus on their water adsorption capacity. The samples were characterized by N2 at 77 K and CO2 at 273 K adsorption isotherms, scanning electron microscopy, transmission electron microscopy and water vapor isotherms at 298, 313 and 328 K. The textural properties of the samples were slightly different: as the ethanol/water ratio increases, the pore volume and specific surface area decrease and the structure of the samples evolves into a well-defined spherical arrangement. In addition, water adsorption capacity of the samples was similar to that of commercial adsorbents used for gas drying at high relative pressures, but significantly lower at low relative pressures. Moreover, varying of the ethanol/water ratio did not lead to a noticeable improvement in the water adsorption capacity at low relative pressures and hence these samples are not suitable for deep gas drying. On the other hand, as they require less energy to be regenerated, HMS are alternatives to be considered in less demanding situations, such as coarse drying and water harvesting from air.
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- 2022
34. Creation of N2-Phobic Morphology of 3d Graphene/Polymer Monolithic Structures for Outstanding Co2/N2 Selectivity
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Iranzu Barbarin, Nikolaos Politakos, Luis Serrano-Cantador, Juan Antonio Cecilia, Oihane Sanz, and Radmila Tomovska
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History ,Polymers and Plastics ,Business and International Management ,Industrial and Manufacturing Engineering - Published
- 2022
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35. Oxidative Condensation of Furfural with Ethanol Using Preformed AU Colloidal Nanoparticles. Impact of Stabilizer and Heat Treatment Protocols on Catalytic Activity and Stability
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Nikolaos Dimitratos, Eleonora Monti, Alessia Ventimiglia, Carolina Alejandra Garcia Soto, Francesca Martelli, Elena Rodríguez-Aguado, Juan Antonio Cecilia, Pedro Maireles-Torres, Francesca Ospitali, Tommaso Tabanelli, Stefania Albonetti, and Fabrizio Cavani
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- 2022
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36. The Role of Copper in the Hydrogenation of Furfural and Levulinic Acid
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Cristina García-Sancho, Josefa María Mérida-Robles, Juan Antonio Cecilia-Buenestado, Ramón Moreno-Tost, and Pedro Jesús Maireles-Torres
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Inorganic Chemistry ,Organic Chemistry ,General Medicine ,Physical and Theoretical Chemistry ,Molecular Biology ,Spectroscopy ,Catalysis ,Computer Science Applications - Abstract
Currently, there is a great interest in the development of sustainable and green technologies for production of biofuels and chemicals. In this sense, much attention is being paid to lignocellulosic biomass as feedstock, as alternative to fossil-based resources, inasmuch as its fractions can be transformed into value-added chemicals. Two important platform molecules derived from lignocellulosic sugars are furfural and levulinic acid, which can be transformed into a large spectrum of chemicals, by hydrogenation, oxidation, or condensation, with applications as solvents, agrochemicals, fragrances, pharmaceuticals, among others. However, in many cases, noble metal-based catalysts, scarce and expensive, are used. Therefore, an important effort is performed to search the most abundant, readily available, and cheap transition-metal-based catalysts. Among these, copper-based catalysts have been proposed, and the present review deals with the hydrogenation of furfural and levulinic acid, with Cu-based catalysts, into several relevant chemicals: furfuryl alcohol, 2-methylfuran, and cyclopentanone from FUR, and γ-valerolactone and 2-methyltetrahydrofuran from LA. Special emphasis has been placed on catalytic processes used (gas- and liquid-phase, catalytic transfer hydrogenation), under heterogeneous catalysis. Moreover, the effect of addition of other metal to Cu-based catalysts has been considered, as well as the issue related to catalyst stability in reusing studies.
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- 2023
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37. Materials Design for N2O Capture: Separation in Gas Mixtures
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Daniel Ballesteros-Plata, Juan Antonio Cecilia, Isabel Barroso-Martín, José Jiménez-Jiménez, Antonia Infantes-Molina, and Enrique Rodríguez-Castellón
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Physical and Theoretical Chemistry ,Catalysis ,General Environmental Science - Abstract
The adsorption of greenhouse gases (GHG) as a method to reduce their emissions into the atmosphere is an alternative that is easier to implement industrially and cheaper than other existing technologies, such as chemical capture, cryogenic separation, or membrane separation. The vast majority of works found in the literature have focused their efforts on capturing CO2 as it is the largest GHG. However, although N2O emissions are not as large as CO2, the impact that N2O has on the stratosphere and climate is much larger in proportion, despite which there is not much research on N2O capture. Since both gases are usually emitted into the atmosphere together (along with other gases), it is necessary to design selective adsorbents capable of capturing and separating these gases from each other and from other gases, to mitigate the effects of climate change. This review aims to compile the existing information to date on porous adsorbents, the characteristics of the N2O adsorption processes and, above all, aims to focus the reader’s gaze on the importance of designing selective adsorbents for greenhouse gas mixtures.
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- 2022
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38. Protein Adsorption onto Modified Porous Silica by Single and Binary Human Serum Protein Solutions
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Diana C. S. Azevedo, Juan Antonio Cecilia, Diego Romao Gondim, Ivanildo J. Silva, Enrique Vilarrasa-García, Enrique Rodríguez-Castellón, and Thaina N. B. Rodrigues
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Diffraction ,purification ,QH301-705.5 ,Article ,Catalysis ,mesocellular foam ,Inorganic Chemistry ,Adsorption ,X-ray photoelectron spectroscopy ,Desorption ,Humans ,human serum: porous silica ,Physical and Theoretical Chemistry ,Biology (General) ,Porosity ,Molecular Biology ,QD1-999 ,Serum Albumin ,Spectroscopy ,Chemistry ,Organic Chemistry ,General Medicine ,Silicon Dioxide ,Blood proteins ,Computer Science Applications ,adsorption isotherm ,SBA-15 ,Chemical engineering ,Serum Globulins ,Porous medium ,Protein adsorption - Abstract
Typical porous silica (SBA-15) has been modified with pore expander agent (1,3,5-trimethylbenzene) and fluoride-species to diminish the length of the channels to obtain materials with different textural properties, varying the Si/Zr molar ratio between 20 and 5. These porous materials were characterized by X-ray Diffraction (XRD), N2 adsorption/desorption isotherms at −196 °C and X-ray Photoelectron Spectroscopy (XPS), obtaining adsorbent with a surface area between 420–337 m2 g−1 and an average pore diameter with a maximum between 20–25 nm. These materials were studied in the adsorption of human blood serum proteins (human serum albumin—HSA and immunoglobulin G—IgG). Generally, the incorporation of small proportions was favorable for proteins adsorption. The adsorption data revealed that the maximum adsorption capacity was reached close to the pI. The batch purification experiments in binary human serum solutions showed that Si sample has considerable adsorption for IgG while HSA adsorption is relatively low, so it is possible its separation.
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- 2021
39. Insights into CO2 adsorption in amino-functionalized SBA-15 synthesized at different aging temperature
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Rafael Morales-Ospino, Moises Bastos-Neto, Enrique Vilarrasa-García, Diana C. S. Azevedo, Enrique Rodríguez-Castellón, and Juan Antonio Cecilia
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Chemistry ,General Chemical Engineering ,02 engineering and technology ,Surfaces and Interfaces ,General Chemistry ,Mesoporous silica ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Co2 adsorption ,Grafting ,01 natural sciences ,0104 chemical sciences ,Amino functionalized ,Adsorption ,Chemical engineering ,Desorption ,Amine gas treating ,0210 nano-technology ,Selectivity - Abstract
Mesoporous silica SBA-15 solids have been synthesized at different aging temperature with the goal of obtaining materials with different textural properties. The synthesized samples have been evaluated for their CO2 adsorption capacity. In order to increase the CO2 adsorption capacity and the CO2/N2 selectivity, the SBA-15 synthesized at different aging temperatures were functionalized via grafting with 3-aminopropyltriethoxysilane (APTES) and via impregnation with polyethyleniminethylenediamine branched (PEI) or tetraethylenepentamine (TEPA). In all cases, the adsorption isotherms of the amine functionalized silica are fitted to the Dualsite-Langmuir model, where physical and chemical adsorption sites are reported. The isotherms reveal that grafted-silicas with APTES displayed the coexistence of both adsorption sites, while the adsorption process of PEI or TEPA impregnated-silicas are mainly governed by chemical interactions. The adsorption isotherms show that the most promising adsorbent for CO2 capture in terms of CO2 adsorption capacity and CO2/N2 selectivity is the SBA synthesized at 393 K (aging temperature) and functionalized with TEPA (50 wt%) (SBA-393-50T). This sample reached a CO2 adsorption capacity of 2.83 mmol g−1 at 100 kPa and 338 K. The CO2 adsorption capacity of this material decreased around 5% after the first adsorption/desorption cycle, maintaining a constant value for successive cycles. SBA-393-50T also showed an outstanding CO2/N2 selectivity, increasing significantly as the CO2 concentration decreases.
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- 2019
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40. Ni supported on sepiolite catalysts for the hydrogenation of furfural to value-added chemicals: influence of the synthesis method on the catalytic performance
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J. J. Quirante-Sánchez, Juan Antonio Cecilia, Pedro Maireles-Torres, Francisco C. Franco, A. Guerrero-Torres, Carmen P. Jiménez-Gómez, and Cristina García-Sancho
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010405 organic chemistry ,Sepiolite ,chemistry.chemical_element ,General Chemistry ,010402 general chemistry ,Furfural ,01 natural sciences ,Catalysis ,0104 chemical sciences ,Furfuryl alcohol ,law.invention ,Nickel ,chemistry.chemical_compound ,chemistry ,law ,Furan ,Calcination ,Selectivity ,Nuclear chemistry - Abstract
Nickel-based catalysts supported on sepiolite catalysts, with a nickel loading between 1 and 10 wt%, have been synthesized by several synthetic strategies (precipitation-deposition, impregnation and grafting-complexation) and subsequent calcination and reduction. The catalysts were characterized by H2 thermoprogrammed reduction (H2-TPR), X-ray diffraction, transmission electron microscopy, N2 adsorption–desorption at − 196 °C, NH3 thermoprogrammed desorption (NH3-TPD) and CO chemisorption. FUR hydrogenation in gas-phase revealed that the most active catalyst was the catalyst synthesized by the grafting-complexation method due to its highest metallic surface area and smallest metal crystal size, reaching a FUR yield close to 85% after 5 h of time-on-stream (TOS) at 190 °C, using a H2:FUR molar ratio of 11.5 and a WHSV of 1.5 h−1. Furan (F), methylfuran (MF) and furfuryl alcohol (FOL); however, the selectivity towards F and MF tend to decrease with the TOS, while FOL selectivity increases.
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- 2019
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41. Selective Production of Furan from Gas-Phase Furfural Decarbonylation on Ni-MgO Catalysts
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Juan Antonio Cecilia, Ramón Moreno-Tost, Carmen P. Jiménez-Gómez, Cristina García-Sancho, and Pedro Maireles-Torres
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Renewable Energy, Sustainability and the Environment ,Chemistry ,General Chemical Engineering ,Decarbonylation ,chemistry.chemical_element ,Ether ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Furfural ,01 natural sciences ,0104 chemical sciences ,Furfuryl alcohol ,Catalysis ,Nickel ,chemistry.chemical_compound ,Yield (chemistry) ,Furan ,Environmental Chemistry ,0210 nano-technology ,Nuclear chemistry - Abstract
A series of Ni-MgO catalysts (Ni/Mg molar ratio: 0.1–0.3), prepared by a coprecipitation-calcination-reduction methodology, was characterized and evaluated in the gas-phase hydrogenation of furfural. In all cases, after reduction at 500 °C, nickel species were present as very tiny metal Ni(0) nanoparticles and forming part as Ni(II) of a NiO-MgO solid solution, as inferred from XRD and XPS techniques. The decarbonylation process of furfural was favored at reaction temperatures as low as 190 °C. The most active catalyst was that with a Ni/Mg molar ratio of 0.25, maintaining a furfural conversion of 96% after 5 h of time-on-stream at 190 °C, by feeding a furfural solution in cyclopentylmethyl ether (5 vol % furfural) under a H2 stream (H2:furfural molar ratio = 11.5 and WHSV = 1.5 h–1). Furan was the main product, with a yield of 88%, whereas furfuryl alcohol was formed at lower reaction temperature and shorter contact time. However, the catalyst suffers a gradual deactivation during a catalytic test of 24 ...
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- 2019
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42. Direct Conversion of Levulinic Acid into Valeric Biofuels Using Pd Supported Over Zeolites as Catalysts
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Juan Antonio Cecilia, Rafael Mariscal, M. López Granados, M. Muñoz-Olasagasti, Pedro Maireles-Torres, and A. Sañudo-Mena
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chemistry.chemical_compound ,Valeric acid ,chemistry ,Yield (chemistry) ,Inorganic chemistry ,Levulinic acid ,General Chemistry ,Fourier transform infrared spectroscopy ,Acetonitrile ,Dispersion (chemistry) ,Catalysis ,Incipient wetness impregnation - Abstract
A series of Pd-based catalysts was prepared by incipient wetness impregnation over different acidic supports: amorphous SiO2-Al2O3, ZSM5 and beta zeolites. In addition to the effect of the support, other variables like the metal loading (0, 1, 2 and 4 wt%) on ZSM5 were tested in the direct conversion of levulinic acid (LA) to valeric biofuels (valeric acid/ester). The best result, a 92% yield of valeric biofuels, was obtained for a 2 wt% Pd supported on ZSM5 catalyst (2PdZSM5) after 8 h of reaction at 240 °C. Characterization techniques such as FTIR spectroscopy (using deuterated acetonitrile and CO as probe molecules), TEM and XPS were employed to explain this catalytic performance. FTIR spectra with deuterated acetonitrile evidenced the moderate acidity (in terms of concentration and strength) of the 2PdZSM5 catalyst, a desirable feature for the proper realization of this reaction. It has been observed that the acidity of the support favors the Pd dispersion, but it is less relevant for its catalytic properties. Finally, the stability of a representative catalyst was demonstrated under flow conditions for over 90 h, obtaining moderate but stable yields for the 2PdZSM5 catalyst.
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- 2019
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43. Oxidative condensation/esterification of furfural with ethanol using preformed Au colloidal nanoparticles. Impact of stabilizer and heat treatment protocols on catalytic activity and stability
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Eleonora Monti, Alessia Ventimiglia, Carolina Alejandra Garcia Soto, Francesca Martelli, Elena Rodríguez-Aguado, Juan Antonio Cecilia, Pedro Maireles-Torres, Francesca Ospitali, Tommaso Tabanelli, Stefania Albonetti, Fabrizio Cavani, Nikolaos Dimitratos, Monti, E, Ventimiglia, A, Soto, CAG, Martelli, F, Rodriguez-Aguado, E, Cecilia, JA, Maireles-Torres, P, Ospitali, F, Tabanelli, T, Albonetti, S, Cavani, F, and Dimitratos, N
- Subjects
Supported Au colloidal nanoparticle ,Effect of stabilizer ,Process Chemistry and Technology ,Ethyl furoate ,Physical and Theoretical Chemistry ,Oxidative condensation ,Furfural ,Furan-2-acrolein ,Catalysis - Abstract
The oxidative condensation of furfural and ethanol has been studied using supported gold colloidal nano particles. The influence of the nature of stabilizer (polyvinylalcohol, polyvinylpyrrolidone), the choice of thermal treatment and washing for removing the stabilizer, on the catalytic performance has been evaluated. Variation of the mean gold particle size and surface coverage of the gold nanoparticles onto the support surface were achieved by modifying the stabilizer to Au weight ratio. Thus, the mean gold particle size was varied in the range of 3-8 nm. The catalytic results showed that the choice of stabilizer, the stabilizer to Au weight ratio, thermal treatment of the catalyst, affect catalytic activity and selectivity/yield to the desired products. When PVA was the chosen stabilizer, the highest yield to furan-2-acrolein (33%) was attained with a PVA to Au weight ratio of 2.4. On the contrary, when PVP was the stabilizer, the best catalytic performance was achieved in its absence, with the yield of furan-2-acrolein reaching 21%. These results showed the strong impact of stabilizer to control catalytic activity and to enhance, in the case of PVA, the yield to the target product, whereas a strong negative effect was observed with PVP. Moreover, a mild thermal treatment of the catalyst and a washing step for the removal of the stabilizer from the catalyst had a positive effect on the catalytic performance.
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- 2022
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44. Effect of Polyvinyl Alcohol Ligands on Supported Gold Nano-Catalysts: Morphological and Kinetics Studies
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Nikolaos Dimitratos, Stefano Scurti, Eleonora Monti, Juan Antonio Cecilia, Elena Rodríguez-Aguado, Daniele Caretti, Scurti S., Monti E., Rodriguez-Aguado E., Caretti D., Cecilia J.A., and Dimitratos N.
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chemistry.chemical_classification ,Gold nanoparticle ,General Chemical Engineering ,Nanoparticle ,hydrogenation of 4-nitrophenol ,Polymer ,Polyvinyl alcohol ,Article ,Catalysis ,Metal ,lcsh:Chemistry ,chemistry.chemical_compound ,chemistry ,X-ray photoelectron spectroscopy ,Dynamic light scattering ,Chemical engineering ,lcsh:QD1-999 ,Colloidal gold ,visual_art ,gold nanoparticles ,visual_art.visual_art_medium ,General Materials Science ,polyvinyl alcohol ligands - Abstract
The effect of polyvinyl alcohol (PVA) stabilizers and gold nanoparticles supported on active carbon (AuNPs/AC) was investigated in this article. Polymers with different molecular weights and hydrolysis degrees have been synthesized and used, like the stabilizing agent of Au nano-catalysts obtained by the sol-immobilization method. The reduction of 4-nitrophenol with NaBH4 has been used as a model reaction to investigate the catalytic activity of synthesized Au/AC catalysts. In addition, we report several characterization techniques such as ultraviolet-visible spectroscopy (UV-Vis), dynamic light scattering (DLS), X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) in order to correlate the properties of the polymer with the metal nanoparticle size and the catalytic activity. A volcano plot was observed linking the catalytic performance with hydrolysis degree and the maximum of the curve was identified at a value of 60%. The Au:PVA-60 weight ratio was changed in order to explain how the amount of the polymer can influence catalytic properties. The effect of nitroaromatic ring substituents on the catalytic mechanism was examined by the Hammett theory. Moreover, the reusability of the catalyst was investigated, with little to no decrease in activity observed over five catalytic cycles. Morphological and kinetic studies reported in this paper reveal the effect of the PVA polymeric stabilizer properties on the size and catalytic activity of supported gold nanoparticles.
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- 2021
45. Microbial Degradation of Lignocellulosic Biomass to Obtain High Value-Added Products
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Pedro Maireles-Torres, Juan Antonio Cecilia, Cristina García-Sancho, and Carmen P. Jiménez-Gómez
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Anaerobic digestion ,business.industry ,Fossil fuel ,food and beverages ,Biomass ,Lignocellulosic biomass ,Environmental science ,Ethanol fermentation ,Microbial biodegradation ,Value added ,business ,Energy source ,Pulp and paper industry - Abstract
The depletion of the fossil fuels has led to the search for and development of more sustainable and environmental benign energy source. In this sense, the biomass has emerged as alternative resource since biomass is the only source from which it is possible to obtain energy and mainly chemicals that, currently, are obtained from the traditional fossil fuels. The selection of the biomass source is a key parameter to reach a sustainable process. Considering these premises, the lignocellulosic biomass has emerged as a potential alternative source due to its non-edible character as well as its high availability throughout the Earth. Traditionally, the lignocellulosic biomass has been treated thermochemically to obtain high value-added products and energy. However, in the recent past, the microbial treatment of the lignocellulosic biomass has emerged as efficient methodology to solve the problems of energy shortage and the synthesis of valuable products. The aim of this chapter is to evaluate the metabolic process involved in the microbial degradation of lignocellulosic biomass as well as highlight the valuable products obtained through this microbial treatment by alcoholic fermentation and anaerobic digestion.
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- 2021
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46. Design of Activated Carbons from the Cellulose Fraction of Agricultural Waste. Applications in Selective Separation and Storage of Gases
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N. Chouikhi, Juan Antonio Cecilia, Enrique Vilarrasa-García, Luis Serrano-Cantador, Sabrine Besghaier, Mohamed Chlendi, Mohamed Bagane, and Enrique Rodriguez Castellon
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- 2021
- Full Text
- View/download PDF
47. Catalytic Applications of Clay Minerals and Hydrotalcites
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Juan Antonio Cecilia and Carmen P. Jiménez-Gómez
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inorganic chemicals ,Materials science ,Hydrotalcite ,020101 civil engineering ,02 engineering and technology ,010402 general chemistry ,lcsh:Chemical technology ,01 natural sciences ,complex mixtures ,Catalysis ,0201 civil engineering ,0104 chemical sciences ,lcsh:Chemistry ,n/a ,Chemical engineering ,lcsh:QD1-999 ,lcsh:TP1-1185 ,Physical and Theoretical Chemistry ,Clay minerals - Abstract
Clay minerals are the most abundant minerals on the surface of Earth [...]
- Published
- 2021
48. Porous SiO2 Nanospheres Modified with ZrO2 and Their Use in One- Pot Catalytic Processes to Obtain Value-Added Chemicals from Furfural
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Juan Antonio Cecilia, Cristina García-Sancho, Ramón Moreno-Tost, Pedro Maireles-Torres, Carmen P. Jiménez-Gómez, Juana M. Rosas, Rocío Maderuelo-Solera, Stefan Richter, and Francisco J. García-Mateos
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Diffraction ,Alcoholes ,Reacciones químicas ,biorefinery ,Materials science ,General Chemical Engineering ,Catalizadores ,Nanopartículas ,General Chemistry ,furfural ,Furfural ,biomass valorization ,Article ,Industrial and Manufacturing Engineering ,Catalysis ,chemistry.chemical_compound ,lignocellulose ,chemistry ,Chemical engineering ,Molar ratio ,porous silica ,Porosity ,Value (mathematics) - Abstract
Porous SiO2 nanospheres have been modified with different proportion of ZrO2 to obtain catalysts with Si/Zr molar ratio between 2.5 and 30. These materials were characterized by X-ray diffraction, transmission electron microscopy, scanning electron microscopy, N2 adsorption-desorption at -196 ºC, X-ray photoelectron spectroscopy and pyridine and 2-6-dimethylpyridine thermoprogrammed desorption. The characterization of these catalysts reveals that the incorporation of a high proportion of Zr favors the formation of Lewis acid sites, which are implied in catalytic transfer hydrogenation processes, whereas the low Brönsted acidity promote dehydration reaction, in such a way that it is possible to obtain a wide range of products from FUR through consecutive reactions, such as furfuryl alcohol, i-propyl furfuryl ether, i-propyl levulinate and γ-valerolactone in a range of temperature of 110-170 ºC between 1-6 h of reaction. Spanish Ministry of Science, Innovation and Universities:RTI2018‐94918‐B‐C44; FEDER (European Union) funds: RTI2018‐94918‐B‐C44 and UMA18-FEDERJA-171; University of Malaga; Junta de Andalucía; Funding for open access charge: Universidad de Málaga/CBUA
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- 2021
49. CO2 Capture by Reduced Graphene Oxide Monoliths with Incorporated CeO2 Grafted with Functionalized Polymer Brushes
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Luis Serrano Cantador, Iranzu Barbarin, Nikolaos Politakos, Juan Antonio Cecilia, and Radmila Tomovska
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Technology ,Materials science ,responsiveness ,QH301-705.5 ,QC1-999 ,polymer brushes ,reduced graphene oxide ,chemistry.chemical_compound ,Adsorption ,poly[(2-(methacryloyloxy)ethyl) trimethylammonium chloride] ,General Materials Science ,Reversible addition−fragmentation chain-transfer polymerization ,Monolith ,Biology (General) ,Instrumentation ,QD1-999 ,cerium oxide ,Acrylic acid ,Fluid Flow and Transfer Processes ,chemistry.chemical_classification ,geography ,geography.geographical_feature_category ,RAFT polymerization ,Process Chemistry and Technology ,Physics ,General Engineering ,Caprolactam ,Chain transfer ,Polymer ,Engineering (General). Civil engineering (General) ,Computer Science Applications ,Chemistry ,chemistry ,Polymerization ,Chemical engineering ,poly(acrylic acid) ,monolith ,TA1-2040 ,CO2 adsorption - Abstract
The monolithic materials of reduced graphene oxide (rGO) can be used successfully in CO2 adsorption. Here, the incorporation of CeO2 particles with and without polymer brushes grafted from the particles showed that the structural properties could be changed, affecting the adsorption of CO2. Polymer brushes of (1) poly(acrylic acid) (PAA), (2) poly(vinyl caprolactam) (PVCL) and (3) poly[(2-(methacryloyloxy)ethyl) trimethylammonium chloride] (PMETAC) were grafted from CeO2 via reversible addition−fragmentation chain transfer (RAFT) polymerization. The preparation of monoliths of rGO with different modified CeO2 particles led to different thermal properties (TGA), structural changes (BET isotherms) and CO2 adsorption. The responsive character of the CeO2@polymer was proven by the DLS and UV results. The responsive character of the particles incorporated into the rGO monolith affected not only the adsorption capacity but also the microstructure and values of the surface volume of the pores of the monolith. Monoliths with porosity values for better adsorption were affected by the responsive character of the polymer. This research was funded by the Basque government, grant number GV IT999-16.
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- 2021
50. Towards functionalized graphene/polymer monolithic structures for selective CO2 capture
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Iranzu Barbarin, Nikolaos Politakos, Luis Serrano-Cantador, Juan Antonio Cecilia, Oihane Sanz, and Radmila Tomovska
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Mechanics of Materials ,General Materials Science ,General Chemistry ,Condensed Matter Physics - Published
- 2022
- Full Text
- View/download PDF
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