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Projeto de investigação
FILTHERCAN: Fluorinated Ionic Liquids-based delivery systems: Biocompatible THERapy for CANcer
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Towards Enhanced Tunability of Aqueous Biphasic Systems
Publication . Carvalho, Sara F.; Custódio, Margarida H.; Pereiro, Ana B.; Araújo, João M. M.; LAQV@REQUIMTE; DQ - Departamento de Química; MDPI - Multidisciplinary Digital Publishing Institute
This work unfolds functionalized ABSs composed of FILs ([C2C1Im][C4F9SO3] and [(Formula presented.)][C4F9SO3]), mere fluoro-containing ILs ([C2C1Im][CF3SO3] and [C4C1Im][CF3SO3]), known globular protein stabilizers (sucrose and [(Formula presented.)][C4F9SO3]), low-molecular-weight carbohydrate (glucose), and even high-charge density salt (K3PO4). The ternary phase diagrams were determined, stressing that FILs highly increased the ability for ABS formation. The functionalized ABSs (FILs vs. mere fluoro-containing ILs) were used to extract lysozyme (Lys). The ABSs’ biphasic regions were screened in terms of protein biocompatibility, analyzing the impact of ABS phase-forming components in Lys by UV-VIS spectrophotometry, CD spectroscopy, fluorescence spectroscopy, DSC, and enzyme assay. Lys partition behavior was characterized in terms of extraction efficiency (% EE). The structure, stability, and function of Lys were maintained or improved throughout the extraction step, as evaluated by CD spectroscopy, DSC, enzyme assay, and SDS-PAGE. Overall, FIL-based ABSs are more versatile and amenable to being tuned by the adequate choice of the phase-forming components and selecting the enriched phase. Binding studies between Lys and ABS phase-forming components were attained by MST, demonstrating the strong interaction between Lys and FILs aggregates. Two of the FIL-based ABSs (30 %wt [C2C1Im][C4F9SO3] + 2 %wt K3PO4 and 30 %wt [C2C1Im][C4F9SO3] + 25 %wt sucrose) allowed the simultaneous purification of Lys and BSA in a single ABS extraction step with high yield (extraction efficiency up to 100%) for both proteins. The purity of both recovered proteins was validated by SDS-PAGE analysis. Even with a high-charge density salt, the FIL-based ABSs developed in this work seem more amenable to be tuned. Lys and BSA were purified through selective partition to opposite phases in a single FIL-based ABS extraction step. FIL-based ABSs are proposed as an improved extraction step for proteins, based on their biocompatibility, customizable properties, and selectivity.
Une étude sociale des techniciens traitant des gaz réfrigérants
Publication . Martinho, Graça; Castro, Paulo J.; Santos, Pedro; Alves, Ana; Araújo, João M. M.; Pereiro, Ana B.; DCEA - Departamento de Ciências e Engenharia do Ambiente; MARE - Centro de Ciências do Mar e do Ambiente; DQ - Departamento de Química; LAQV@REQUIMTE; Elsevier
Compliance with the international agreements and regulations aiming at mitigating emissions of gases with high global warming potential (GWP) requires the involvement of all stakeholders in the value chain of equipment containing refrigeration gases. In particular, the technicians dealing with the installation, maintenance, and dismantling of refrigeration equipment have a relevant role in the prevention of the release of refrigerant gases and their correct management. Besides technical information and training, the awareness of these technicians about the effects of fluorinated gases (F-gases) on global warming is critical for policy, regulations and strategies related to F-gases. This work presents the results of a questionnaire conducted with 586 Portuguese, Spanish, and French technicians to diagnose their behaviours, knowledge, and risk perception face to refrigeration gases and global warming. The results reveal that the repaired equipment mostly contains the pure HFCs R-32 and R-134a, the HFC blends R-410A, R-407C, and R-404A, and the fourth-generation HFC[sbnd]HFO blend R-449A. They also indicate the need to implement more efficient and credible information/awareness campaigns and to improve the training of these professionals in key respects, such as the relation between F-gases and climate change and the importance of their individual responsibility. Several suggestions were provided by the inquired technicians to improve the repair/maintenance process aiming at mitigating the effect of refrigeration gases on climate change, and to improve the awareness of this topic. These suggestions should be taken into consideration to improve legislation and policies.
Coconut shell derived activated carbon for effective separation of greenhouse gases
Publication . Sosa, Julio E.; Ribeiro, Rui P. P. L.; Matos, Inês; Bernardo, Maria; Fonseca, Isabel M.; Mota, José P. B.; Araújo, João M. M.; Pereiro, Ana B.; DQ - Departamento de Química; LAQV@REQUIMTE; Elsevier
The development of efficient adsorbent materials for the selective capture of greenhouse gases (GHGs) is crucial. The porosity and surface area of the materials are key factors for the GHGs separation. This study demonstrates how waste from coconut shell (CS) biomass can be used to design novel biomaterials (CS-CO2, CS-ZnCl2) with enhanced GHG selectivity. A comparison with activated carbon monoliths (ACM) and a metal-organic framework (Fe-BTC) was carried out to assess the impact of different porous matrices on GHGs capture. The adsorption equilibrium of R-32, R-125, R-134a, R-143a, CO2, and CH4 on these materials was measured between 283.15–323.15 K. The adsorption isotherms obtained were fitted using the dual-site Langmuir model. For R-32, R-125, R-134a and R-143a, the adsorption capacity follows ACM > CS-ZnCl2 > Fe-BTC > CS-CO2 due to the decrease of the surface area. The CO2 adsorption capacity is ACM > Fe-BTC > CS-ZnCl2 > CS-CO2, which is related to the micropore volume. In this case, CS-CO2 has a smaller adsorption capacity but is similar to ACM and outperforms Fe-BTC at P < 0.4 MPa. The selectivity of R-410A, R-407C, R-404A, and CO2/CH4 blends was determined with the Ideal Adsorbed Solution Theory (IAST). CS-ZnCl2 shows a higher selectivity for R-125 over R-32 in R-410A and R-407C separations due to its larger pore volume. CS-CO2 predominantly adsorbs R-134a and R-143a over R-125 in R-404A separation. ACM preferentially adsorbs CO2 over CH4 due to its large, elongated micropores. This study introduces innovative materials that improve GHGs separation and help reduce emissions.
Simultaneous Purification of Human Interferon Alpha-2b and Serum Albumin Using Bioprivileged Fluorinated Ionic Liquid-Based Aqueous Biphasic Systems
Publication . Carvalho, Sara F.; Pereiro, Ana B.; Araújo, João M. M.; LAQV@REQUIMTE; DQ - Departamento de Química; MDPI - Multidisciplinary Digital Publishing Institute
Interferon alpha-2b (IFN- (Formula presented.) 2b) is an essential cytokine widely used in the treatment of chronic hepatitis C and hairy cell leukemia, and serum albumin is the most abundant plasma protein with numerous physiological functions. Effective single-step aqueous biphasic system (ABS) extraction for the simultaneous purification of IFN- (Formula presented.) 2b and BSA (serum albumin protein) was developed in this work. Effects of the ionic liquid (IL)-based ABS functionalization, fluorinated ILs (FILs; [C (Formula presented.) C (Formula presented.) Im][C (Formula presented.) F (Formula presented.) SO (Formula presented.)] and [N (Formula presented.)][C (Formula presented.) F (Formula presented.) SO (Formula presented.)]) vs. mere fluoro-containing IL ([C (Formula presented.) C (Formula presented.) Im][CF (Formula presented.) SO (Formula presented.)]), in combination with sucrose or [N (Formula presented.)][H (Formula presented.) PO (Formula presented.)] (well-known globular protein stabilizers), or high-charge-density salt K (Formula presented.) PO (Formula presented.) were investigated. The effects of phase pH, phase water content (%wt), phase composition (%wt), and phase volume ratio were investigated. The phase pH was found to have a significant effect on IFN- (Formula presented.) 2b and BSA partition. Experimental results show that simultaneous single-step purification was achieved with a high yield (extraction efficiency up to 100%) for both proteins and a purification factor of IFN- (Formula presented.) 2b high in the enriched IFN- (Formula presented.) 2b phase (up to 23.22) and low in the BSA-enriched phase (down to 0.00). SDS-PAGE analysis confirmed the purity of both recovered proteins. The stability and structure of IFN- (Formula presented.) 2b and BSA were preserved or even improved (FIL-rich phase) during the purification step, as evaluated by CD spectroscopy and DSC. Binding studies of IFN- (Formula presented.) 2b and BSA with the ABS phase-forming components were assessed by MST, showing the strong interaction between FILs aggregates and both proteins. In view of their biocompatibility, customizable properties, and selectivity, FIL-based ABSs are suggested as an improved purification step that could facilitate the development of biologics.
Hydrophobic Eutectogels for the Removal of Contaminants of Emerging Concern from Water
Publication . Gabirondo, Elena; Araújo, Joao M. M.; Pereiro, Ana B.; Tomé, Liliana C.; LAQV@REQUIMTE; DQ - Departamento de Química; Wiley | Wiley-VCH Verlag
Five hydrophobic eutectic solvents based on menthol and thymol were prepared and incorporated into a poly(ethylene glycol) diacrylate (PEGDA) network to form eutectogel membranes. The two most promising eutectogels were further optimized by adding ethyl hexylacrylate (HA) to the eutectogel formulation to improve the compatibility between the eutectic solvent and polymer network and to enhance the water resistance of the resulting membranes. Thermal analysis confirmed the successful formation and integration of eutectic solvents within the polymer network. Rheological studies demonstrated the rubber-like behavior of the prepared hydrophobic eutectogels, with menthol-based variants exhibiting superior mechanical properties. Finally, sorption experiments were conducted using the optimized octanoic acid:menthol PEGDA-HA eutectogel to evaluate its efficiency in removing various contaminants of emerging concern (CECs), including diclofenac, iopromide, cefazolin, bisphenol A, and dichlorophenol. The results revealed high sorption capacities for bisphenol A (3213 mg⋅kg−1) and dichlorophenol (2981 mg⋅kg−1), followed by diclofenac (1490 mg⋅kg−1), whereas minimal sorption capacities were observed for iopromide and cefazolin. Overall, this study demonstrates the potential of hydrophobic eutectogels as efficient and tunable materials for water purification, paving the way for their application in the environmental remediation of different emerging pollutants related to global change and human activities.
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Fundação para a Ciência e a Tecnologia
Programa de financiamento
CEEC IND4ed
Número da atribuição
2021.01432.CEECIND/CP1657/CT0044