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1.
Gels ; 10(7)2024 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-39057475

RESUMEN

Solid-state supercapacitors with gel electrolytes have emerged as a promising field for various energy storage applications, including electronic devices, electric vehicles, and mobile phones. In this study, nanocomposite gel membranes were fabricated using the solution casting method with perfluorosulfonic acid (PFSA) ionomer dispersion, both with and without the incorporation of 10 wt.% montmorillonite (MMT). MMT, a natural clay known for its high surface area and layered structure, is expected to enhance the properties of supercapacitor systems. Manganese oxide, selected for its pseudocapacitive behavior in a neutral electrolyte, was synthesized via direct co-precipitation. The materials underwent structural and morphological characterization. For electrochemical evaluation, a two-electrode Swagelok cell was employed, featuring a carbon xerogel negative electrode, a manganese dioxide positive electrode, and a PFSA polymer membrane serving as both the electrolyte and separator. The membrane was immersed in a 1 M Na2SO4 solution before testing. A comprehensive electrochemical analysis of the hybrid cells was conducted and compared with a symmetric carbon/carbon supercapacitor. Cyclic voltammetric curves were recorded, and galvanostatic charge-discharge tests were conducted at various temperatures (20, 40, 60 °C). The hybrid cell with the PFSA/MMT 10 wt.% exhibited the highest specific capacitance and maintained its hybrid profile after prolonged cycling at elevated temperatures, highlighting the potential of the newly developed membrane.

2.
Gels ; 10(2)2024 Feb 02.
Artículo en Inglés | MEDLINE | ID: mdl-38391453

RESUMEN

This study deals with the preparation of adsorbents from a commercial xerogel by chemically modifying its surface with concentrated mineral acids and alkali metal chlorides, their physicochemical characterization, and their use as adsorbents for gallic acid in aqueous solution. Although there are publications on the use of carbon xerogels as adsorbents, we propose and study simple modifications that can change their chemical properties and, therefore, their performance as adsorbents. The adsorbate of choice is gallic acid and, to our knowledge, there is no history of its adsorption with carbon xerogels. The prepared adsorbents have a high specific surface area (347-563 m2 g-1), better pore development for samples treated with alkali metal chlorides than with mineral acids, and are more acidic than the initial xerogel (p.z.c range 2.49-6.87 vs. 7.20). The adsorption equilibrium is reached in <16 h with a kinetic constant between 0.018 and 0.035 h-1 for the pseudo-second-order model. The adsorption capacity, according to the Langmuir model, reaches 62.89 to 83.33 mg g-1. The adsorption properties of the commercial xerogel improved over a wide range of pH values and temperatures. The experimental results indicate that the adsorption process is thermodynamically favored.

3.
Gels ; 9(12)2023 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-38131969

RESUMEN

For the development and optimization of solid-state symmetrical supercapacitors, herein, we propose using carbon-based electrodes and sodium- and lithium-form Aquivion electrolyte membranes, which serve as the separator and electrolyte. Carbon xerogels, synthesized using microwave-assisted sol-gel methodology, with designed and controlled properties were obtained as electrode materials. Commercial activated carbon (YP-50F, "Kuraray Europe" GmbH) was used as the active material for comparison. Notably, the developed solid-state symmetrical supercapacitors provide sufficiently high specific capacitances of 105-110 F g-1 at 0.2 A g-1, along with an energy density of 4.5 Wh kg-1 at 300 W kg-1, and a voltage window of 0-1.2 V in aqueous environments, also demonstrating an excellent cycling stability for up to 10,000 charge/discharge cycles. These results can demonstrate the potential applications of carbon xerogel as the active electrode material and cation exchange membrane as the electrolyte in the development of solid-state supercapacitor devices.

4.
Gels ; 9(11)2023 Oct 31.
Artículo en Inglés | MEDLINE | ID: mdl-37998958

RESUMEN

Multifunctional materials based on carbon xerogel (CX) with embedded bismuth (Bi) and iron (Fe) nanoparticles are tested for ultrasensitive amperometric detection of lead cation (Pb2+) and hydrogen peroxide (H2O2). The prepared CXBiFe-T nanocomposites were annealed at different pyrolysis temperatures (T, between 600 and 1050 °C) and characterized by X-ray diffraction (XRD), Raman spectroscopy, N2 adsorption, dynamic light scattering (DLS), and electron microscopies (SEM/EDX and TEM). Electrochemical impedance spectroscopy (EIS) and square wave anodic stripping voltammetry (SWV) performed at glassy carbon (GC) electrodes modified with chitosan (Chi)-CXBiFe-T evidenced that GC/Chi-CXBiFe-1050 electrodes exhibit excellent analytical behavior for Pb2+ and H2O2 amperometric detection: high sensitivity for Pb2+ (9.2·105 µA/µM) and outstanding limits of detection (97 fM, signal-to-noise ratio 3) for Pb2+, and remarkable for H2O2 (2.51 µM). The notable improvements were found to be favored by the increase in pyrolysis temperature. Multi-scale parameters such as (i) graphitization, densification of carbon support, and oxide nanoparticle reduction and purification were considered key aspects in the correlation between material properties and electrochemical response, followed by other effects such as (ii) average nanoparticle and Voronoi domain dimensions and (iii) average CXBiFe-T aggregate dimension.

5.
Materials (Basel) ; 16(19)2023 Oct 05.
Artículo en Inglés | MEDLINE | ID: mdl-37834703

RESUMEN

Carbon xerogels (CXs) are materials obtained via the pyrolysis of resins prepared via the sol-gel polycondensation of resorcinol and formaldehyde. These materials attract great attention as adsorbents, catalyst supports, and energy storage materials. One of the most interesting features of CXs is the possibility of fine-tuning their structures and textures by changing the synthesis conditions in the sol-gel stage. Thus, the first part of this review is devoted to the processes taking place in the polycondensation stage of organic precursors. The formation of hydroxymethyl derivatives of resorcinol and their polycondensation take place at this stage. Both of these processes are catalyzed by acids or bases. It is revealed that the sol-gel synthesis conditions, such as pH, the formaldehyde/resorcinol ratio, concentration, and the type of basic modifier, all affect the texture of the materials being prepared. The variation in these parameters allows one to obtain CXs with pore sizes ranging from 2-3 nm to 100-200 nm. The possibility of using other precursors for the preparation of organic aerogels is examined as well. For instance, if phenol is used instead of resorcinol, the capabilities of the sol-gel method become rather limited. At the same time, other phenolic compounds can be applied with great efficiency. The methods of gel drying and the pyrolysis conditions are also reviewed. Another important aspect analyzed within this review is the surface modification of CXs by introducing various functional groups and heteroatoms. It is shown that compounds containing nitrogen, sulfur, boron, or phosphorus can be introduced at the polycondensation stage to incorporate these elements into the gel structure. Thus, the highest surface amount of nitrogen (6-11 at%) was achieved in the case of the polycondensation of formaldehyde with melamine and hydroxyaniline. Finally, the methods of preparing metal-doped CXs are overviewed. Special attention is paid to the introduction of a metal precursor in the gelation step. The elements of the iron subgroup (Fe, Ni, Co) were found to catalyze carbon graphitization. Therefore, their introduction can be useful for enhancing the electrochemical properties of CXs. However, since the metal surface is often covered by carbon, such materials are poorly applicable to conventional catalytic processes. In summary, the applications of CXs and metal-doped CXs are briefly mentioned. Among the promising application areas, Li-ion batteries, supercapacitors, fuel cells, and adsorbents are of special interest.

6.
Environ Sci Pollut Res Int ; 30(43): 98211-98230, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37606781

RESUMEN

This paper proposes the study of a solar-based photocatalytic ozonation process for the degradation of salicylic acid (SA) using a novel S-scheme ZnO/Cu2O/CuO/carbon xerogel photocatalyst. The incorporation of CuO and Cu2O aims to enhance charge mobility through the formation of p-n heterojunctions with ZnO, whereas the carbon xerogel (XC) was selected due to its eco-friendly nature, capacity to stabilize S-scheme heterojunctions as a solid-state electron mediator, and ability to function as a reducing agent under high temperatures. The characterization of the composites demonstrates that the presence of the XC during the calcination step led to the reduction of a fraction of the CuO into Cu2O, forming a ternary semiconductor heterojunction system. In terms of photocatalysis, the XC/ZnO-CuxO 5% composite achieved the best efficiency for salicylic acid degradation, mainly due to the stabilization of the S-scheme charge transfer pathway between the ZnO/CuO/Cu2O semiconductors by the XC. The total organic carbon (TOC) removal during heterogeneous photocatalysis was 80% for the solar-based process and 68% for the visible light process, after 300 min. The solar-based photocatalytic ozonation process was highly successful regarding the degradation of SA, achieving a 75% increase in the apparent reaction rate constant when compared to heterogeneous photocatalysis. Furthermore, a 78% TOC removal was achieved after 150 min, which is half the time required by the heterogeneous photocatalysis to obtain the same result. Temperature, salinity, and turbidity had major effects on the efficiency of the photocatalytic ozonation process; the system's pH did not cause any major performance variation, which holds relevance for industrial applications.


Asunto(s)
Ozono , Óxido de Zinc , Temperatura , Salinidad , Carbono , Ácido Salicílico , Concentración de Iones de Hidrógeno
7.
Chemosphere ; 333: 138915, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-37172623

RESUMEN

N-Nitrosamines are one of the environmentally significant byproducts from aqueous amine-based post-combustion carbon capture systems (CCS) due to their potential risk to human health. Safely mitigating nitrosamines before they are emitted from these CO2 capture systems is therefore a key concern before widescale deployment of CCS can be used to address worldwide decarbonization goals. Electrochemical decomposition is one viable route to neutralize these harmful compounds. The circulating emission control waterwash system, commonly installed at the end of the flue gas treatment trains to minimize amine solvent emissions, plays an important role to capture N-nitrosamines and control their emission into the environment. The waterwash solution is the last point where these compounds can be properly neutralized before becoming an environmental hazard. In this study, the decomposition mechanisms of N-nitrosamines in a simulated CCS waterwash with residual alkanolamines was investigated using several laboratory-scale electrolyzers utilizing carbon xerogel (CX) electrodes. H-cell experiments revealed that N-nitrosamines were decomposed through a reduction reaction and are converted into their corresponding secondary amines thereby neutralizing their environmental impact. Batch-cell experiments statistically examined the kinetic models of N-nitrosamine removal by a combined adsorption and decomposition processes. The cathodic reduction of the N-nitrosamines statistically obeyed the first-order reaction model. Finally, a prototype flow-through reactor using an authentic waterwash was used to successfully target and decompose N-nitrosamines to below the detectable level without degrading the amine solvent compounds allowing them to be return to the CCS and lower the system operating costs. The developed electrolyzer was able to efficiently remove greater than 98% of N-nitrosamines from the waterwash solution without producing any additional environmentally harmful compounds and offers an effective and safe route to mitigate these compounds from CO2 capture systems.


Asunto(s)
Dióxido de Carbono , Nitrosaminas , Humanos , Dióxido de Carbono/química , Aminas/química , Nitrosaminas/química , Carbono , Solventes/química
8.
Environ Sci Pollut Res Int ; 30(12): 34684-34697, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36515879

RESUMEN

Organic xerogel microspheres (SX) were synthesized by inverse emulsion sol-gel polymerization and carbonized to obtain carbon xerogel spheres (SXCs). The catalyst was K2CO3 or Fe(C2H3O2)2, and the clay sodium sepiolite (SNa) or exfoliated vermiculite (Vexf) was added during the synthesis. Depending on the catalyst and clays, the SXCs were designated SXC-K, SXC-Fe, Vexf-K, Vexf-Fe, SNa-Fe, and SNa-K. At pH = 7 and T = 25 °C, the SXCs' adsorption capacities towards diclofenac (DCF) in water increased as follows: SXC-K < Vexf-Fe < SXC-Fe < SNa-Fe < SNa-K < Vexf-K and this order is associated with the SXCs' surface area and mesopore volume. The Vexf-K displayed the highest capacity for DCF due to its optimal textural and chemical properties, and the DCF maximum uptake was 560 mg/g at pH = 6 and T = 35 °C. The adsorption capacity towards Cd2+ and Pb2+ decreased as SX-K > SX-Fe > SXC-K > SXC-Fe, indicating that the non-carbonized materials (SX) presented higher adsorption capacity than the SXCs because the SXs had a higher acidic site content. Adding SNa or Vexf to SXs enhanced the adsorption capacity towards Cd(II), and SNa-SX-K presented an exceptionally high capacity of 182.7 mg/g. This synergistic effect revealed that the Cd2+ was adsorbed on the SX-K acidic sites and by cation exchange on the SNa.


Asunto(s)
Metales Pesados , Contaminantes Químicos del Agua , Arcilla , Diclofenaco/química , Microesferas , Cadmio , Metales Pesados/química , Agua , Adsorción , Contaminantes Químicos del Agua/química
9.
Molecules ; 27(23)2022 Dec 02.
Artículo en Inglés | MEDLINE | ID: mdl-36500576

RESUMEN

Recent studies on the removal of pollutants via adsorption include the use of carbon-based adsorbents, due to their high porosity and large surface area; however, such materials lack photoactive properties. This study evaluates the synergistic effect of integrated mesoporous carbon xerogel (derived from resorcinol formaldehyde) and titanium dioxide (TiO2) for combined adsorption and photodegradation application. The complex formed between carbon xerogel and TiO2 phase was investigated through FTIR, proving the presence of a Ti-O-C chemical linkage. The physicochemical properties of the synthesised adsorbent-photocatalyst were probed using FESEM, BET analysis and UV-Vis analysis. The kinetics, equilibrium adsorption, effect of pH, and effect of adsorbent dosage were investigated. The expansion of the absorbance range to the visible range was verified, and the corresponding band gap evaluated. These properties enabled a visible light response when the system was exposed to visible light post adsorption. Hence, an assistive adsorption-photodegradation phenomenon was successfully executed. The adsorption performance exhibited 85% dye degradation which improved to 99% following photodegradation. Further experiments showed the reduction of microorganisms under visible light, where no microbial colonies were observed after treatment, indicating the potential application of these composite materials.


Asunto(s)
Contaminantes Ambientales , Fotólisis , Titanio/química , Adsorción , Carbono , Catálisis
10.
Materials (Basel) ; 15(7)2022 Mar 25.
Artículo en Inglés | MEDLINE | ID: mdl-35407762

RESUMEN

Hierarchical porous carbons are known to enhance the electrochemical features of electrodes in electrochemical capacitors. However, the contribution of surface oxygen and the resulting functionalities and wettability, along with the role of electrical conductivity and degree of amorphous or crystalline nature in the micro-mesoporous carbons, are not yet clear. This article considers the effect of carbonisation temperature (500-900 °C) and the type of activation (CO2, KOH) on the properties mentioned above in case of carbon xerogels (CXs) to understand the resulting electrochemical performances. Depending on the carbonisation temperature, CX materials differ in micropore surface area (722-1078 m2 g-1) while retaining a mesopore surface area ~300 m2 g-1, oxygen content (3-15%, surface oxygen 0-7%), surface functionalities, electrical conductivity (7 × 10-6-8 S m-1), and degree of amorphous or crystalline nature. Based on the results, electrochemical performances depend primarily on electrical conductivity, followed by surface oxygen content and meso-micropore connectivity. The way of activation using a varied extent of CO2 exposure and KOH concentrations played differently in CX in terms of pore connectivity from meso- to micropores and their contributions and degree of oxidation, and resulted in different electrochemical behaviours. Such performances of activated CXs depend solely on micro-mesopore features.

11.
Materials (Basel) ; 14(18)2021 Sep 13.
Artículo en Inglés | MEDLINE | ID: mdl-34576486

RESUMEN

Layered double hydroxides (LDHs) have emerged as promising electrodes materials for the methanol oxidation reaction. Here, we report on the preparation of different LDHs with the hydrothermal process. The effect of the divalent cation (i.e., Ni, Co, and Zn) on the electrochemical performance of methanol oxidation was investigated. Moreover, nanocomposites of LDHs and carbon xerogels (CX) supported on nickel foam (NF) substrate were prepared to investigate the role of carbon xerogel. The results show that NiFe-LDH/CX/NF is an efficient electrocatalyst for methanol oxidation with a current density that reaches 400 mA·m-2 compared to 250 and 90 mA·cm-2 for NiFe-LDH/NF and NF, respectively. In addition, all LDH/CX/NF nanocomposites show excellent stability for methanol oxidation. A clear relationship is observed between the electrodes crystallite size and their activity to methanol oxidation. The smaller the crystallite size, the higher the current density delivered. Additionally, the presence of carbon xerogel in the nanocomposites offer 3D interconnected micro/mesopores, which facilitate both mass and electron transport.

12.
Polymers (Basel) ; 13(16)2021 Aug 07.
Artículo en Inglés | MEDLINE | ID: mdl-34451171

RESUMEN

Carbon/carbon (C/C) composite xerogels dried by evaporation were prepared in this study to observe the change of their porous properties and their morphology by nitrogen sorption apparatus and a scanning electron microscope. Resorcinol and formaldehyde (RF) sols as a matrix phase and cotton fibers (CF) as a dispersed phase were mixed and gelated to be CF/RF composite hydrogels. The composite hydrogels were exchanged by t-butanol (TBA), dried by evaporation at 50 °C, and carbonized at 1000 °C to become the C/C composite xerogels. The results show that the CF addition does not decrease the mesoporous properties of the C/C composite xerogels. Moreover, the CF addition can alleviate the pore shrinkage, and it can maintain the mesopore structure. The mesopore size and the micropore size of C/C composites are insignificantly changed because the CF addition and the solvent exchange using TBA may suppress the pore shrinkage despite the gas-liquid interface existing during the evaporation drying.

13.
Materials (Basel) ; 13(21)2020 Oct 31.
Artículo en Inglés | MEDLINE | ID: mdl-33142879

RESUMEN

Introducing new inexpensive materials for supercapacitors application with high energy density and stability, is the current research challenge. In this work, Silver doped carbon xerogels have been synthesized via a simple sol-gel method. The silver doped carbon xerogels are further surface functionalized with different loadings of nickel cobaltite (1 wt.%, 5 wt.%, and 10 wt.%) using a facile impregnation process. The morphology and textural properties of the obtained composites are characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and nitrogen physisorption analysis. The silver doped carbon xerogels display a higher surface area and larger mesopore volume compared to the un-doped carbon xerogels and hierarchically porous structure is obtained for all materials. The hybrid composites have been utilized as electrode materials for symmetric supercapacitors in 6 M KOH electrolyte. Among all the hybrid composites, silver doped carbon xerogel functionalized with 1 wt.% nickel cobaltite (NiCo1/Ag-CX) shows the best supercapacitor performance: high specific capacitance (368 F g-1 at 0.1 A g-1), low equivalent series resistance (1.9 Ω), high rate capability (99% capacitance retention after 2000 cycles at 1 A g-1), and high energy and power densities (50 Wh/Kg, 200 W/Kg at 0.1 A g-1). It is found that the specific capacitance does not only depend on surface area, but also on others factors such as particle size, uniform particle distribution, micro-mesoporous structure, which contribute to abundant active sites and fast charge, and ion transfer rates between the electrolyte and the active sites.

14.
Nanomaterials (Basel) ; 10(9)2020 Sep 10.
Artículo en Inglés | MEDLINE | ID: mdl-32927755

RESUMEN

Molybdenum carbide (Mo2C)-based electrocatalysts were prepared using two different carbon supports, commercial carbon nanotubes (CNTs) and synthesised carbon xerogel (CXG), to be studied from the point of view of both capacitive and electrocatalytic properties. Cation type (K+ or Na+) in the alkaline electrolyte solution did not affect the rate of formation of the electrical double layer at a low scan rate of 10 mV s-1. Conversely, the different mobility of these cations through the electrolyte was found to be crucial for the rate of double-layer formation at higher scan rates. Molybdenum carbide supported on carbon xerogel (Mo2C/CXG) showed ca. 3 times higher double-layer capacity amounting to 75 mF cm-2 compared to molybdenum carbide supported on carbon nanotubes (Mo2C/CNT) with a value of 23 mF cm-2 due to having more than double the surface area size. The electrocatalytic properties of carbon-supported molybdenum carbides for the oxygen reduction reaction in alkaline media were evaluated using linear scan voltammetry with a rotating disk electrode. The studied materials demonstrated good electrocatalytic performance with Mo2C/CXG delivering higher current densities at more positive onset and half-wave potential. The number of electrons exchanged during oxygen reduction reaction (ORR) was calculated to be 3, suggesting a combination of four- and two-electron mechanism.

15.
Materials (Basel) ; 13(16)2020 Aug 10.
Artículo en Inglés | MEDLINE | ID: mdl-32785141

RESUMEN

A series of carbon xerogels doped with cobalt, nickel, and iron have been prepared through the sol-gel method. The doped carbon xerogels were further functionalized with binary and ternary transition metal oxides containing Co, Ni, and Zn oxides by the hydrothermal method. A development in the mesopore volume is achieved for functionalized carbon xerogel doped with iron. However, in the functionalization of carbon xerogel with ternary metal oxides, a reduction in pore diameter and mesopore volume is found. In addition, all functionalized metal oxides/carbon are in the form of 3D nanobundles with different lengths and widths. The prepared samples have been tested as electrocatalysts for oxygen reduction reaction (ORR) in basic medium. All composites showed excellent oxygen reduction reaction activity; the low equivalent series resistance of the Zn-Ni-Co/Co-CX composite was especially remarkable, indicating high electronic conductivity. It has been established that the role of Zn in this type of metal oxides nanobundles-based ORR catalyst is not only positive, but its effect could be enhanced by the presence of Ni.

16.
ACS Appl Mater Interfaces ; 12(32): 36054-36065, 2020 Aug 12.
Artículo en Inglés | MEDLINE | ID: mdl-32692145

RESUMEN

The present study elucidates the role of surface oxygen functional groups on the electrochemical behavior of porous carbons when used as anodes for Li-ion batteries. To achieve this objective, a carbon xerogel (CX) obtained by pyrolysis of a resorcinol-formaldehyde gel, was modified by different postsynthesis treatments in order to modulate its surface chemistry while maintaining its external surface constant. Various surface modifications were obtained by oxidation in air, in situ polymerization of dopamine, and finally by grafting of a polyethylene oxide layer on the polydopamine coating. While oxidation in air did not affect the pore texture of the CX, modifications by coating techniques substantially decreased the micropore fraction. Detailed electrochemical characterizations of the materials processed as electrodes were performed by capacitance measurements and galvanostatic cycling. Surface chemistry results, from X-ray photoelectron spectroscopy, show that the accessibility and the capacity increase when carbonyl (R-C═O) groups are formed on the CX, but not with oxides and hydroxyls. The amount of surface carbonyls, and in particular, aldehyde (O═CH) groups, is found to be the key parameter because it is directly correlated with the modified CX electrochemical behavior. Overall, the explored surface coatings tend to reduce the micropore volume and add mainly hydroxyl functional groups but hardly change the Li+ insertion/deinsertion capacities, while oxidation in air adds carbonyl groups, increasing the Li+ ion storage capacity, thanks to an improved accessibility to the carbon network, which is not caused by any textural change.

17.
J Colloid Interface Sci ; 565: 368-377, 2020 Apr 01.
Artículo en Inglés | MEDLINE | ID: mdl-31981846

RESUMEN

The present work reports a rapid, tunable synthesis of resorcinol-formaldehyde (RF) carbon xerogels and their potential application as anode materials for lithium-ion battery. An iron-containing deep eutectic solvent (DES) is applied as both reaction medium and catalyst for the polymerization and graphitization. Water at different levels is employed as a co-solvent to mediate the polymerization and phase separation processes to produce a more-developed porous structure. The established binary-solvent synthesis strategy greatly simplifies the RF carbon xerogel preparation processes with a very short sol-gel time and a more acceptable ambient pressure drying. A duplex carbon configuration of rich microporosity (SBET = 566 m2 g-1) and expanded nanographite is achieved in the binary-solvent system with a DES mass fraction of 70%. The integrated structural merit is highly favorable for lithium storage, showing a reversible capacity of 633 mA h g-1 at 0.1 A g-1 and an excellent rate performance (205 mA h g-1 at 5 A g-1) as well as superior cycling stability.

18.
Environ Technol ; 41(27): 3534-3543, 2020 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-31046640

RESUMEN

The study examined the preparation, characterization and the use of carbon xerogel (CX) material for the adsorption of three model naphthenic acids (NAs); such as, heptanoic acid (HPA), 5-cyclohexanepentanoic acid (CHPA), and 5-phenylvaleric acid (PVA). CX was synthesized by sol-gel method from resorcinol and formaldehyde. The characterization results showed that CX was a mesoporous material with large surface area (573 m2/g) and high pore volume (1.55 cm3/g), which was mainly composed of carbon (93.20%) and oxygen (6.71%). Adsorption studies revealed that PVA, the NA having an aromatic ring was adsorbed more easily by CX (87 mg/g) due to π-π interactions, followed by HPA (65 mg/g) and CHPA (61 mg/g). In addition, by studying the effect of solution pH, the result confirmed that repulsion greatly hindered the adsorption of HPA onto CX at pHs above that of the pHPZC and at lower pHs attractive electrostatic forces promoted adsorption. Adsorption kinetics fitted the pseudo-first-order model, which suggested that physisorption was most likely the means of adsorption. For the intraparticle diffusion model, the rate of film diffusion was higher than the rate of pore diffusion for each model compound regardless of their structure. Accordingly, this confirmed that pore diffusion was the rate-limiting step, although film diffusion still maintained a significant role in the rate of diffusion. In general, CX exhibited excellent adsorption performance due to its highly mesoporous character so it could be used as a passive treatment method in tailing ponds for removal of organic matters.


Asunto(s)
Carbono , Contaminantes Químicos del Agua , Adsorción , Ácidos Carboxílicos , Cinética
19.
Molecules ; 24(18)2019 Sep 19.
Artículo en Inglés | MEDLINE | ID: mdl-31546753

RESUMEN

The main objective of this study is to develop a novel dual-purpose material based on carbon xerogel microspheres (CXMs) that permits the delayed release of cannabidiol (CBD) and the removal of aflatoxin. The CXMs were prepared by the sol-gel method and functionalized with phosphoric acid (CXMP) and melamine (CXMN). The support and the modified materials were characterized by scanning electronic microscopy (SEM), N2 adsorption at -196 °C, X-ray photoelectron spectroscopy (XPS), and zeta potential. For the loading of the cannabidiol (CBD) in the porous samples, batch-mode adsorption experiments at 25 °C were performed, varying the concentration of CBD. The desorption kinetics was performed at two conditions for simulating the gastric (pH of 2.1) and intestinal (pH of 7.4) conditions at 37 °C based on in vitro CBD release. Posteriorly, the samples obtained after desorption were used to study aflatoxin removal, which was evaluated through adsorption experiments at pH = 7.4 and 37 °C. The adsorption isotherms of CBD showed a type I(b) behavior, with the adsorbed uptake being higher for the support than for the modified materials with P and N. Meanwhile, the desorption kinetics of CBD at gastric conditions indicated release values lower than 8%, and the remaining amount was desorbed at pH = 7.4 in three hours until reaching 100% based on the in vitro experiments. The results for aflatoxin showed total removal in less than 30 min for all the materials evaluated. This study opens a broader landscape in which to develop dual-purpose materials for the delayed release of CBD, improving its bioavailability and allowing aflatoxin removal in gastric conditions.


Asunto(s)
Aflatoxinas/aislamiento & purificación , Cannabidiol/farmacología , Carbono/química , Microesferas , Adsorción , Preparaciones de Acción Retardada/farmacología , Cinética , Nitrógeno/química , Electricidad Estática , Temperatura
20.
Water Res ; 154: 402-411, 2019 05 01.
Artículo en Inglés | MEDLINE | ID: mdl-30822600

RESUMEN

This study illustrated the preparation, characterization and the use of carbon xerogel materials for the adsorption of acid-extractable fractions (AEF) and naphthenic acids (NAs) from oil sands process water (OSPW). Adsorption results demonstrated that the mesoporous carbonaceous material can successfully be used to adsorb persistent and toxic organic contaminants from OSPW. Carbon xerogel (CX) made at pH 5.5 showed high surface area (573 m2/g) and removed a larger amount of AEF than CX made at pH 6.9 (391 m2/g). The adsorption equilibrium was reached by 24 h for both AEF and classical NAs. 74.6% of AEF and 88.8% of classical NAs were removed by CX5.5 during 24-h adsorption. With respect to classical NAs, a larger the carbon number resulted in higher NA removal. Carbon number had more influence on NA removal when compared with hydrogen deficiency resulting from rings or unsaturated bonding formation (-Z number). The equilibrium adsorption capacity was found to be 15 mg AEF/g and 7.8 mg NAs/g for CX5.5. Adsorption of AEF and classical NAs onto CX5.5 followed pseudo-second order kinetics. With respect to diffusion of AEF and NAs, there were three distinct diffusion regions: bulk, film and pore. Pore diffusion had the lowest rate constant in all cases analyzed and was thus the rate limiting step. The results of this study showed that a mesoporous carbonaceous material such as CX may have the potential to be utilized in a fixed bed adsorption/filtration systems for continuous treatment of OSPW or as a semi-passive treatment method in pit lakes for the removal of organic constituents from OSPW.


Asunto(s)
Yacimiento de Petróleo y Gas , Contaminantes Químicos del Agua , Adsorción , Carbono , Ácidos Carboxílicos , Filtración
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