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This work reports the preparation of zeolite hydrogel composite (ZHC) based on κ-carrageenan (KC) and AQSOA-Z05 zeolite and its potential use in water remediation applications for methylene blue (MB) dye adsorption. The ZHC was synthesized via the graft-copolymerization technique using the crosslinked hydrogel of KC as polymer matrix. Effects of in...
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The use of some hydrogels as adsorbents for pollutants removal from wastewater is limited due to their high swelling properties and the difficulty in recovering them after the adsorption process. To overcome these problems, a new hydrogel nanocomposite based on chitosan-grafted-polyacrylic acid/oxidized electrospun carbon nanofibers (CT-g-PAA/O-ECN...
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... They have shown that the entrapment of zeolite particles into a porous polymer network was a promising pathway toward overcoming their drawbacks. The combinations of zeolites with some other polymers (poly(dimethylsiloxane) (Adnadjevic and Jovanovic, 2000;Adnadjević et al., 1997), poly(vinyl alcohol) (Viboonratanasri et al., 2021), chitosan (Swaghatha and Cindrella, 2022), polyimide (Li et al., 2020), polysulfone/polyimide (Muntha et al., 2018), polyethylene (Marinković et al., 2022;Marinkovic et al., 2019), xanthan gum-alginate (Zhang et al., 2014), poly(lactic acid) (Yuzay et al., 2010), κ-carrageenan-poly(acrylamide-co-methacrylic acid) (Mittal et al., 2020a), starch-g-poly(acrylic acid) (Zhang et al., 2016), etc.) have been also proposed but rarely in the form of composite hydrogels. Although in most of these composites the idea was not to use zeolites as solely reinforcing fillers, but also as active components and even activity carriers, in the majority of reported literature only up to 10 wt% of zeolite was possible to be embedded in polymeric matrices. ...
... Still, to the best of our knowledge there are only a couple of studies where higher zeolite concentrations were embedded in polymeric networks. Supramolecular spatial organization (structure) of PMAA hydrogels and polymeric composites with zeolites has been investigated in the following works (Junior et al., 2020;Mittal et al., 2020a;Yan et al., 2014;Yuzay et al., 2010;Zhang et al., 2016Zhang et al., , 2017. Yuzay et al. (2010) have determined that the introduction of LTA zeolite in poly(lactic acid) led to the enhanced nuclearization of PLA and the increase in the crystallinity of the composite. ...
... Crystal architectures of LTA zeolite have been also retained after integration in alginate and xanthan gum-alginate biopolymers (Zhang et al., 2014). Investigating the structure of the κ-carrageenan-poly(acrylamide-co-methacrylic acid)/AQSOA-Z05 zeolite hydrogel composites, Mittal et al. (2020a) have concluded that the AQSOA-Z05 zeolite particles were successfully incorporated within the employed polymeric matrix in the way of the wrapping of zeolite particles between different polymeric chains indicating the growth of hydrogel polymer around zeolite particles. Junior et al. (2020) have determined that the structures of the PMAA hydrogel and its composites with laponite were predominantly amorphous, but with domains with ordering at very small interplane distances, the so called short-range order, that correspond to 2θ = 15.5 • and 2θ = 30.7 • reflections in XRD patterns. ...
... The reason for the weak adsorption capacity in the acidic field is the presence of hydrogen ions H + of a large amount that competes with the dye molecules for adsorption sites (Mittal, Al Alili and Alhassan, 2020). In addition, clay is more affected by these ions due to the properties of clay, that differs from activated carbon in terms of the nature of the charges on its surface (Adeyemo, Adeoye and Bello, 2017). ...
Activated carbon and natural clay are extremely promising for the removal of dyes in a water solution. Natural clay and activated carbon were characterized using X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FTIR) techniques, and the food dye was characterized by UV-Visible. The effects of various experimental parameters, such as initial carmine concentration, contact time, temperature and pH were studied. The removal of the dye increases with the decrease in the initial concentration of carmine and the contact time of the solution. The percentage of carmine removal increases accordingly, reaching 97% for activated carbon and 67% for natural clay. Langmuir and Freundlich adsorption models were used for the adsorption equilibrium descriptions. The data was very well corrected with these models. Monolayer adsorption capacities were equal to 31 mgg-1 at pH 8.0 and 27°C. Adsorption measurements show that the adsorption process is very fast and physical in nature. Thermodynamic parameters such as enthalpy ∆H°, ∆S° entropy and ∆G° free enthalpy were also evaluated to reveal the nature of adsorption. The results explain that the adsorption process is an exothermic, spontaneous physisorption.
... Exploration of various kinds of interactions existing among the protein/amino acid-surfactant systems has attracted the interest of many academic researchers around the globe by virtue of their wide applications in foods and cosmetics, detergency, biosciences, drug delivery, and biotechnological processes [1][2][3][4][5][6][7]. The drug delivery application is the most appealing of them because different amino acid-surfactant combinations can be used to modulate drug distribution [8][9][10][11]. ...
Molecular interactions present between 1-pentadecyl-3-methylimidazolium bromide and the biologically important amino acid additives (glycine, l-alanine, and l-valine) have been examined in aqueous media by employing conductivity, UV–Visible, refractive index, and FT-IR spectroscopy at different compositions and temperatures. Furthermore, using the electrical conductivity data, critical micelle concentration, degree of counter-ion dissociation, and various thermodynamic parameters of micellization have been computed. To study the interactions in the micellar system, the effects of additives on these parameters have been carefully analyzed. UV–Visible and refractive index are carried out to outline the results stated above, along with FT-IR results to confirm the various interactions prevailing in the system.
Graphical Abstract
... The WAC of NIP M-βCD: CA NSs (237%) was higher than the NIP βCD: CA NSs (126%), as it is presented in Table 3. This could be explained by the fact that the native cyclodextrin (CD) is 10-fold less soluble than the M-βCD: CA, as it was presented in the literature [87,88]. The presence of methyl groups could affect the structure of the nanosponge, and thus the water absorption capacity also. ...
Melatonin is a neurohormone that ameliorates many health conditions when it is administered as a drug, but its drawbacks are its oral and intravenous fast release. To overcome the limitations associated with melatonin release, cyclodextrin-based nanosponges (CD-based NSs) can be used. Under their attractive properties, CD-based NSs are well-known to provide the sustained release of the drug. Green cyclodextrin (CD)-based molecularly imprinted nanosponges (MIP-NSs) are successfully synthesized by reacting β-Cyclodextrin (β-CD) or Methyl-β Cyclodextrin (M-βCD) with citric acid as a cross-linking agent at a 1:8 molar ratio, and melatonin is introduced as a template molecule. In addition, CD-based non-molecularly imprinted nanosponges (NIP-NSs) are synthesized following the same procedure as MIP-NSs without the presence of melatonin. The resulting polymers are characterized by CHNS-O Elemental, Fourier Transform Infrared Spectroscopy (FTIR), Thermogravimetric (TGA), Differential Scanning Calorimetry (DSC), Zeta Potential, and High-Performance Liquid Chromatography (HPLC-UV) analyses, etc. The encapsulation efficiencies are 60–90% for MIP-NSs and 20–40% for NIP-NSs, whereas melatonin loading capacities are 1–1.5% for MIP-NSs and 4–7% for NIP-NSs. A better-controlled drug release performance (pH = 7.4) for 24 h is displayed by the in vitro release study of MIP-NSs (30–50% released melatonin) than NIP-NSs (50–70% released melatonin) due to the different associations within the polymeric structure. Furthermore, a computational study, through the static simulations in the gas phase at a Geometry Frequency Non-covalent interactions (GFN2 level), is performed to support the inclusion complex between βCD and melatonin with the automatic energy exploration performed by Conformer-Rotamer Ensemble Sampling Tool (CREST). A total of 58% of the CD/melatonin interactions are dominated by weak forces. CD-based MIP-NSs and CD-based NIP-NSs are mixed with cream formulations for enhancing and sustaining the melatonin delivery into the skin. The efficiency of cream formulations is determined by stability, spreadability, viscosity, and pH. This development of a new skin formulation, based on an imprinting approach, will be of the utmost importance in future research at improving skin permeation through transdermal delivery, associated with narrow therapeutic windows or low bioavailability of drugs with various health benefits.
Keywords: cyclodextrin; molecularly imprinted nanosponges; non-moleculary imprinted nanosponges; melatonin; cream formulation; computational study
... Acetone and sodium bicarbonate were taken as porogens. MBA and 1, 4-butanediol diacrylate were taken as crosslinking agents (Disha et al. 2016;Mittal et al. 2018Mittal et al. , 2020Saruchi et al. 2013). ...
The present work deals with the synthesis of biodegradable hydrogel of a natural polysaccharide aloe vera and vinyl monomer acrylic acid. In this synthesis, ammonium persulfate–glutaraldehyde was used as initiator-cross-linker system, acrylic acid as monomer and aloe vera as backbone. Grafting was confirmed by different techniques like SEM, FT-IR, XRD and EDS. Maximum percentage swelling of synthesized hydrogel was found to be 756%. Biodegradation behavior of synthesized hydrogel [Av-cl-poly(AA)] was studied by soil burial, composting and vermicomposting methods. Maximum biodegradation was found to be 90%, 94% and 93% in case of soil burial, composting and vermicomposting methods, respectively. Biodegradation of Av-cl-poly(AA) was confirmed by FT-IR and SEM techniques. Water retention capacity was prolonged from 11 to 20 days using synthesized Av-cl-poly(AA). Water content of clay soil and sandy loam soil was increased to an extent of 6.1% and 5.79%, respectively. Synthesized Av-cl-poly(AA) has been found to be effective in sustained release of harmful pesticide dichlorvos. The results showed that maximum release of dichlorvos was found to be 1024.34 ppm after 44 h.
... Methylene blue is a basic dye or cationic dye that is very toxic if its concentration exceeds 1 mg L −1 in the aquatic environment (Oladoye et al. 2022). MB dye has been classified as a hazardous compound for humans, fauna, and flora (Mittal et al. 2020). As for inorganic pollutants, copper (Cu 2+ ), despite its many advantages, is considered a very toxic heavy metal, even at diluted concentrations (Kouassi et al. 2022). ...
The current study aims to evaluate the effectiveness of mesoporous fly ash (M-FA) as an efficient adsorbent in treating an aqueous solution contaminated by methylene blue (MB) dye. The mesoporous fly ash was also used in a newly developed geopolymer synthesis strategy to immobilize hazardous compounds such as methylene blue and copper (Cu2+) from aqueous media. X-ray diffraction (XRD), Fourier-transformed infrared spectroscopy (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Brunauer–Emmett–Tellet (BET), and zero charge analysis were used to characterize the mineralogical structure, functional group, surface morphology, surface area, and surface charge of M-FA material, respectively. The batch study experiments like contact time, initial dye concentration, pH solution, and temperature are varied to attain good removal efficiency. The results of the isothermal model were consistent with the Langmuir model. The pseudo-first-order (PFO), pseudo-second-order (PSO), and intraparticle diffusion (IPD) models were applied to analyze the kinetic data, with the PSO model indicating a strong correlation coefficient. The thermodynamic study showed that the adsorption of dye onto the M-FA material was non-spontaneous and endothermic. The leaching assay revealed that the M-FA-based geopolymer exhibits a favorable potential to immobilize both the organic dye and the heavy metal, as the findings of the UV–Visible spectroscopy reflected that MB dye and Cu metal were not present in all aqueous media during the different contact times. Finally, this study made it clear that fly ash can be used as a low-cost adsorbent for aqueous media treatment and can be also employed for the immobilization of hazardous substances through a geopolymerization process.
... In another example the synthesis of hydrogel composite (ZHC) using κ-CG and AQSOA-Z05 zeolite was performed by Mittal et al. [123]. The prepared ZHC hydrogel was applied for remediation of water through the elimination of MB dye. ...
The need to replace renewable polymers such as marine-based resources with non-biodegradable, plastic polymers has increased due to environmental issues. Carrageenan is a phycocolloid derived from Irish Moss or carrageenan moss, a type of red algae, mainly Chondrus crispus from which the name carrageenan is derived. Due to the wide variety of algae, they can be extracted from, there are variations in the structures of carrageenan, developed from a basic linear sulfated galactose chain. It performs diverse valuable roles through its aptitude to maintain great amounts of water, being able to form a gel at room temperature, metal chelating, and activities. Carrageenan revealed potential bioactive properties, like immunomodulatory, antiviral, antibacterial, anticoagulant, antioxidant, and antitumor actions. As mentioned, this polymer has hydrogel formation capacity, and its gelling ability is applied in various fields such as pharmaceutical sciences, food technology, biotechnology, engineering, etc. This review contains exhaustive information regarding carrageenan structures, extraction methods, the gel formation mechanism, properties, and the recent development in biomedical and environmental applications of carrageenan-based hydrogels. The biomedical applications comprise wound healing, drug delivery, and tissue engineering. In the field of environmental applications, these hydrogels are employed in the elimination of varied aqueous contaminants like dyes, drugs, metals, etc. at the end of the review, several existing challenges and prospects are also described.
Graphical Abstract
... In a study, the preparation of zeolite hydrogel composite (ZHC) based on κ-carrageenan (KC) and AQSOA-Z05 zeolite and its potential use in water remediation applications for methylene blue (MB) dye adsorption. The ZHC was synthesized via the graft-copolymerization technique using the cross-linked hydrogel of KC as a polymer matrix [23]. The hydrophilic structure of hydrogels allows water to easily diffuse through them, and dyes dissolved in water can interact with the functional groups of the hydrogels. ...
For hazardous dye removal, this research developed a promising adsorbent based on chitosan (CH) and sodium alginate (ALG) nanocomposite modified with graphene oxide (GO) and bentonite (BN). The amphoteric characteristics of the obtained nanocomposite with both positive and negative charges were used to exclude anionic and cationic dyes from waste aqueous solutions. The synthesized nanocomposite was characterized by XRD, FTIR, FESEM, and reaction parameters were optimized to compare the swelling capacity of both the synthesized nanocomposite. The adsorption capacity of CH/ALG/GO and CH/ALG/BN nanocomposites was compared by adsorbing the xylenol orange (XO) (anionic) and methylene blue (MB) (cationic) dye. For MB removal, CH-ALG-GO nanocomposite adsorbed 91% with 0.5 g whereas CH-ALG-BN adsorbed 96% with 0.5 g adsorbent dose in neutral pH solution. For XO removal, CH-ALG-GO nanocomposite adsorbed 85% with 0.5 g whereas CH-ALG-BN adsorbed 93% with 0.5 g adsorbent dose in neutral pH solution. The resultant porous nanocomposite can effectively remove cationic and anionic dyes such as methylene blue (MB) and xylenol orange (XO) from wastewater. With adsorption maxima of 0.731 mg/g and 0.195 mg/g, respectively, the CH-ALG-BN nanocomposite was able to remove both cationic dye (MB) and anionic dye (XO) as an adsorbent.
Graphical Abstract
... Natural gums-based hydrogels can also be further modified by incorporating different fillers such as metal oxide nanoparticle (MO NPs) [9,63,126,[136][137][138][139], clays [106,140,141], zeolites [101,142] and GO [74,135] within the polymer matrix. The incorporation of these filers within the hydrogel matrix improve their mechanical and surface properties but at the same time also provides addition adsorption sites for the attachment of pollutants. ...
... Due to the presence of different functional groups in the structure of zeolites, they also showed promising results as adsorbents for the treatment of dye contaminated wastewater [147,148]. The hydrogel composites of natural gums with different zeolites were synthesized having the properties and benefits of both zeolites as well as polysaccharides [101,142]. Hydrogel composites of Zeolite-Y with the graft co-polymer of gum karaya and poly(NIPAM-co-AA) were synthesized by incorporating and homogeneously dispersing zeolite particles within the hydrogel matrix [101]. Synthesized hydrogel composite was used as an adsorbent to remove BG dye particles from wastewater. ...
Freshwater scarcity is one of the world's foremost environmental stress concerns. In the last few years, with sustainable industrial growth and rapidly growing population, the problem of freshwater shortage has encouraged researchers to conduct comprehensive research for the development of advanced water harvesting and wastewater treatment techniques. Natural gums-based hydrogels have been widely used in different water purification and harvesting applications because of their environment friendly nature, high water absorption, adsorption and retention capacities. In this article, we presented an entirely conceptual and critical review of literature mainly focused on the potential of different natural gums-based hydrogel in water harvesting and wastewater treatment applications. First, different categories of natural gums-based hydrogels including stimuli responsive hydrogels, physically and chemically crosslinked hydrogels, were introduced. Then, the emphasis was given on the role of natural gums-based hydrogels in different wastewater treatment applications like adsorption, photocatalysis and flocculation. After that, the latest research progress on the use of natural gums-based hydrogels in atmospheric water harvesting and seawater desalination was discussed. Finally, different challenges and main limitations associated with the use of natural gums-hydrogels in water purification and harvesting applications were discussed to understand the research gaps and drawbacks which need improvements.
... The change in morphological characteristics of the parent polymer upon undergoing cationic graft co-polymerization was investigated using FESEM analysis. The FESEM images revealed the uniform and smooth surface of the polymeric backbone with the small dents and grooved surfaces disseminated throughout the XG surface [44] shown in Fig. 5a. However, the morphology of grafted co-polymer viz. ...
A new synthetic protocol has been devised for the preparation of polysaccharide-based grafted Copolymers which offers the grafted gels with high % grafting and substantial swelling properties which may provide a great overlook for environmental remediation applications by eradication of various lethal contaminants from the aqueous system. Herein, thionyl chloride facilitated cationic polymerization have been reported, which acts as an initiator as well as polymerizing agent for the synthesis of xanthan gum (XG) grafted acrylamide (AAM), N,N-dimethyl acrylamide (DMA), N-hydroxymethyl acrylamide (HMA) and acrylic acid (AA) Copolymers and the resulted grafted Copolymers are designated as XAAM, XDMA, XHMA and XAA respectively. The successful synthesis of grafted Copolymers was established from spectral, morphological, and thermal analysis. BET analysis revealed the upsurge in surface area and pore size of grafted Copolymers as compared to virgin XG. The synthesized grafted Copolymers showed the appreciable adsorption capability towards synthetic dyes. The XAAM showed the 99% and 97% adsorption for cationic malachite green (MG) and anionic solochrome black T (SBT) with 119.27 mg/g and 122.67 mg/g adsorption capacity respectively. Thermodynamic studies confirmed the endothermic nature of adsorption process and followed pseudo-second-order kinetics model. The present report divulges that thionyl chloride facilitated cationic polymerization is a promising protocol for the preparation of vinyl monomers based XG grafted Copolymers which can serve as an effectual adsorbent for the environmental remediation.
Graphical Abstract
