Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 22
Filtrar
Mais filtros










Base de dados
Intervalo de ano de publicação
1.
Chemosphere ; 352: 141213, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38336040

RESUMO

Discharge of textile dye effluents into water bodies is creating stress to aquatic life and contaminating water resources. In this study, a new biopolymer adsorbent silk fibroin (SF) was prepared from Bombyx mori silk fibroin (SF) and used for removal of Solochrome Black-T (SB-T) from water. This innovative adsorbent exhibits an exceptional adsorption capacity of 20.08 mg/g, achieving a removal efficiency of approximately 98.6 % within 60 min. Notably, the powdered SF adsorbent demonstrates rapid kinetics, surpassing the performance of previously reported similar adsorbents in adsorption capacity and reaction speed. The molecular weight and particle diameter of the material were observed to be > 1.243 kDa and 3 µm, respectively. The experimental investigations were performed on different parameters, viz., adsorbent dosage, contact time, repeatability, and desorption-adsorption study. The experimental data well fit for the Langmuir model (R2 = 0.937, qmax = 20.08 mg/g) and the pseudo-second-order kinetics (R2 = 0.921 and qe = 1.496 mg/g). Compared to the adsorbents reported in the literature, the newly prepared SF showed high adsorption capacity and faster kinetics to address real-life situations. The novelty of this work extends beyond its remarkable adsorption capabilities. The SF adsorbent offers a cost-effective, sustainable solution and regenerable adsorption material with minimal negative environmental impacts. This regenerability, with its versatility and broad applicability, positions powdered SF fibroin as a transformative technology in water treatment and environmental protection.


Assuntos
Bombyx , Fibroínas , Poluentes Químicos da Água , Purificação da Água , Animais , Seda , Pós , Adsorção , Cinética , Concentração de Íons de Hidrogênio
2.
Environ Res ; 207: 112198, 2022 05 01.
Artigo em Inglês | MEDLINE | ID: mdl-34656635

RESUMO

Microfibers (MFs) in aquatic and marine ecosystems adsorb toxic heavy metals and then transfer the heavy metals enriched MFs to living organisms. In this research paper, the adsorption-desorption dynamics of heavy metals onto MFs was studied by using theoretical models and experimental investigations. The adsorption of metals onto MFs was well correlated for the Freundlich model and the adsorption kinetics follows pseudo-second order rate equation. The adsorption capacity of naturally weathered MFs was 30.8 mg g-1 which is about 35% higher than the synthetic fiber of similar range of size of MFs. The leaching of heavy metals from MFs was found that 90-95% of adsorbed metals were leached within 24 h. The leaching of Ti(II) and Al(III) were slower than the other metal ions. The salinity has shown decrease in adsorption capacity of MFs for heavy metals. Based on the Nemerov pollution index (PN), the naturally weathered MFs enriched with heavy metals in sediments became heavily polluted with PN values between 2.98 and 3.49. The risk index value of 396 represents that the bottom dwellers and other marine organisms in the Narmada estuary high risk from MFs and MFs enriched with metals. This study indicates that MFs play dominant role in fate and distribution of heavy metals in the estuarine ecosystems.


Assuntos
Metais Pesados , Poluentes Químicos da Água , Adsorção , Ecossistema , Monitoramento Ambiental , Estuários , Sedimentos Geológicos , Metais Pesados/análise , Poluentes Químicos da Água/análise
3.
Sci Total Environ ; 816: 151522, 2022 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-34752862

RESUMO

The newly prepared reduced graphene oxide-MnO2 (rGO-MnO2) nanocomposite has exhibited highly selective CO2 adsorption from gaseous mixtures at elevated temperatures. The Mn2+ basic sites are scattered over the rGO-MnO2 nanocomposite which produce an effective BET surface area of 710 m2 g-1 for selective CO2 capture. The selective adsorption of CO2 (5.87 mmol g-1) over N2 (0.36 mmol g-1) and CH4 (0.41 mmol g-1) at 298 K/1 bar was achieved by the nanocomposite. The heat of adsorption followed a unique correlation with the quantity of CO2 adsorbed and fits well to the Fowler-Guggenheim equation. The mechanism of CO2 adsorption on the nanocomposite was complemented with molecular modelling and simulations. The rGO-MnO2 have shown better CO2 adsorption capacity of 28.5 mmol g-1 at 323 K/20 bar as compared to zeolite derivatives, MOFs, and carbons as reported in the literature. The formation of inert frameworks with 3-6 nm porous structure in the nanocomposite thermally stabilizes to capture CO2 repeatedly. The nanocomposite with adsorption capacity of 3.69 mmol g-1 at 373 K/1 bar is quite close to real-life conditions for flue gas treatment.

4.
Sci Rep ; 11(1): 17321, 2021 08 27.
Artigo em Inglês | MEDLINE | ID: mdl-34453094

RESUMO

A complex of reduced graphene oxide (rGO) and fluorescein (FL) dye nanoparticles of size between 50 and 100 nm has been prepared and its sensing performance for detection of As(III) in drinking water has been reported. When As(III) binds to the rGO-FL nanoparticles the relative quenching of fluorescence was increased with increase in As(III) concentration thus provide two linear calibration ranges (0-4.0 mmol L-1 and 4.0-10 mmol L-1). The fluorescence quenching mechanism was investigated by using time-resolved fluorescence spectroscopy and molecular modeling. The detection limit of this sensor has been determined as equal to 0.96 µg L-1 which is about 10 times lower than the WHO stipulated standard for As(III) in drinking water (10 µg L-1). The analytical performance and potential application of the nanosensor was compared to commercial field kits used in arsenic monitoring. The sensor proposed in this study is fast, sensitive and accurate for detection of As(III) in drinking water and environmental samples.

5.
Chemosphere ; 284: 131405, 2021 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-34225122

RESUMO

Cenospheres (CS) are spherical shaped inorganic frameworks present in with fly ash which is generated from coal-fired thermal power plants. These spherical structures were functionalized with imidazole and amine moieties to capture CO2 selectively from flue gases at elevated temperature. The functionalized CS have shown a high selectivity for CO2 adsorption (4.68 mmol g-1) over N2 (0.46 mmol g-1) at 333 K/1 bar from a simulated flue gas (0.15 CO2 and 0.85 N2, v%) composition of thermal power plants. When the moisture content reached to 30 vol% the adsorption capacity of CS materials was reduced to 20 vol% as compared to dry flue gas. The functionalized CS can be used repeatedly for 50 cycles without losing its adsorption capacity. The cost estimate for CO2 capture by using the proposed adsorption system would be $12.01/ton of CO2 which is lower as compared to amine absorption system and zeolite-based adsorption system reported in the literature. The CS materials are prepared from solid wastes reduce the cost of production and their large scale manufacturing is technically feasible to capture CO2 from industrial flue gases efficiently in near future.


Assuntos
Cinza de Carvão , Resíduos Sólidos , Dióxido de Carbono , Cinza de Carvão/análise , Centrais Elétricas , Temperatura
6.
Mater Sci Eng C Mater Biol Appl ; 121: 111864, 2021 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-33579494

RESUMO

The design and preparation of clinically relevant endodontic obturating material for root canal therapy is a great challenge. For the first time, we report a new polymer nanocomposite which was prepared by using reversible addition-fragmentation chain-transfer (RAFT) polymerization of methacrylic acid and methylene glycol dimethacrylate. The polymer was embedded with reduced graphene oxide nanoplatelets (rGO). These graphene nanoplatelets were embedded in the polymers (GNPs) have shown the tensile strength (27--36%) and the elongation at break 2.1 - 3.1% is quite similar to the commercial gutta percha (GP-C). Atomic force micrograph provided interesting information related to scattering of rGO flakes in GNPs and the surface of GNP contains crystalline spikes of height varied between 0.95 and 1.26 µm. These spikes improved the adhesion of GNPs to bio-interface. The GNPs were 95% more effective in inhibiting bacterial colonization without disturbing the nearby cell integrity compared to commercial GP. It was found that the GNPs after incubation of 24 h at 37 °C, the radius of the inhibition zone was 6.8 mm and 4.3 mm for E.coli and S. aureus, respectively indicating better effective antibacterial activity than the GP-C. This work offers biocompatible, better adhesive and antibacterial endodontic obturating material for future root canal therapy.


Assuntos
Grafite , Materiais Restauradores do Canal Radicular , Guta-Percha , Polímeros , Obturação do Canal Radicular , Tratamento do Canal Radicular , Staphylococcus aureus
7.
Talanta ; 219: 121273, 2020 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-32887163

RESUMO

A highly sensitive sensor based on molecularly imprinted polymer film was devised for determination of polycyclic aromatic hydrocarbon (PAHs) in aquatic solutions. In this paper we report, electro-polymerisation of 4-vinyl pyridine (4VP) and target, pyrene, using cyclic voltammeter in electrolyte medium, forming the pyrene imprinted polymer. After polymerisation, the pyrene was removed from imprinted polymer using methanol to produce sensory nanofilm characterised by infrared spectrometer, optical and atomic force microscopy. The mechanism of nanofilm sensing was established using atomic models and electrochemical response by differential pulse voltammeter with the redox system of ([Fe(CN)6]3-/[Fe(CN)6]4-). The π-π interaction between pyrene and 4VP was primary cause for pyrene recognition in aqueous solutions and the model binding score for this interaction was -5.10 kcal mol-1. The electrochemical sensor determined pyrene in the concentration range of 1 × 10-4 - 1 ng L-1, resulting best linear regression (r2 > 0.9) and detection limit of 0.001 ng L-1. The recovery percentage of pyrene from the nanofilm was 83-110% in water samples and the imprinting factor value was 2.67. Therefore, the novel imprinted polymer nanofilm sensor showed highest sensitivity for target pyrene in aqueous samples compared to reported sensors.


Assuntos
Impressão Molecular , Técnicas Eletroquímicas , Limite de Detecção , Microscopia de Força Atômica , Polimerização , Polímeros
8.
J Hazard Mater ; 398: 122994, 2020 11 05.
Artigo em Inglês | MEDLINE | ID: mdl-32504956

RESUMO

Abundance of microplastics in aquatic and marine ecosystems is contaminating the seafood and it is leading to transfer of toxic pollutants to human beings. In this article, we report the hazardous nature and cancer risk of microplastics which originate from e-waste. Capture of carcinogenic polycyclic aromatic hydrocarbons (PAHs) onto microplastics by adsorption phenomena and an assessment of probable cancer risk of ingested PAHs enriched microplastics by human beings have been investigated. The adsorption equilibrium was well fit for the Freundlich isotherm model. The adsorption capacity of carcinogenic PAHs on microplastics was ranged from 46 to 236 µg g-1 and the maximum binding was achieved within 45 min in water. The leachate derived from microplastics of e-waste were highly hazardous in nature, for example, the sum of PAHs was 3.17 mg L-1 which is about 1000 times higher than the standard for benzo[a]pyrene, a congener of PAHs. The calculated cancer risk in terms of lifetime of microplastic ingestion would be 1.13 × 10-5 for children and 1.28 × 10-5 for adults and these values are higher than the recommended value of 106. The abundance of microplastics could transfer hazardous pollutants to seafood (e.g., fishes and prawns) leading to cancer risk in human beings.


Assuntos
Neoplasias , Hidrocarbonetos Policíclicos Aromáticos , Poluentes Químicos da Água , Adulto , Animais , Criança , Ecossistema , Monitoramento Ambiental , Humanos , Microplásticos , Neoplasias/induzido quimicamente , Neoplasias/epidemiologia , Plásticos/toxicidade , Hidrocarbonetos Policíclicos Aromáticos/análise , Hidrocarbonetos Policíclicos Aromáticos/toxicidade , Medição de Risco , Poluentes Químicos da Água/análise , Poluentes Químicos da Água/toxicidade
9.
Mater Sci Eng C Mater Biol Appl ; 110: 110672, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-32204100

RESUMO

In this article for the first time, we have reported, a facile way for the creation of E.coli impressions in the polymer for selective capture and to destroy E. coli in drinking water. This microporous imprinted polymer has shown the existence of micrometer size rod shape cavities with the population of 2.45 × 102 ± 60 imprints per cm2. Adsorption capacity of the polymer for E.coli was 103 CFU mg-1. This microporous imprinted polymer captured 99% of the bacteria within 30 min at initial concentration of 109 CFU mL-1. The non-imprinted polymer prepared without the bacteria imprinting reported only 40% of the bacteria removal even after 60 min. The reduced graphene oxide was embedded in the microporous imprinted polymer and it reported minimum inhibitory concentration at 7.4 mg L-1. Within 10 min, reduced graphene oxide completely kills the E.coli while microporous imprinted polymer was embedded with the reduced graphene oxide takes about 13 min to disinfect the water. The reduced graphene oxide nanoparticles were near the imprinted cavity to generate localized temperature between 180 and 210 °C to kill the bacterial cells trapped inside the imprinted cavities of the polymer. The thermal atomic force microscope with the specialized heated probe tips were used to determine the localized temperature in the polymers. The localized thermal energy would be responsible for the production of superoxides, which were as similar to photolysis reactions, and would be further improving antibacterial activity. The combination of selective capture and destruction of pathogens in a single molecular construct improves disinfection of drinking water.


Assuntos
Água Potável/microbiologia , Escherichia coli/efeitos dos fármacos , Grafite/farmacologia , Impressão Molecular , Adsorção , Antibacterianos/farmacologia , Desinfecção , Concentração de Íons de Hidrogênio , Testes de Sensibilidade Microbiana , Nitrogênio/química , Oxirredução , Espectroscopia Fotoeletrônica , Eletricidade Estática , Propriedades de Superfície
10.
Mater Sci Eng C Mater Biol Appl ; 99: 222-230, 2019 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-30889694

RESUMO

In this article, a new approach to directly synthesize drug molecule imbedded in the nanometer sized polymer particles is reported. Molecular imprinting is used to prepare polymers for drug specific for selectively loading of a desired drug. Computer simulations were performed to provide mechanistic insights on the binding modalities of model cancer drug, amygdalin with the polymer precursors. Controlled release of amygdalin from nanoMIPs was studied in vitro cell test and monitoring the absorbance at λem of 390 nm by fluorescence. The nanoparticles imprinted with amygdalin (nanoMIPs) showed high drug loading (0.98 mg g-1) and also releases drug in a controlled way without burst release. The polymer releases amygdalin 0.095 µg (5 min), 0.120 µg (30 min), 0.180 µg (180 min), 0.205 µg in 300 min in de-ionized water and similar pattern of release was observed in buffer 2 and 7. The sustained release of drug from nanoMIPs follows Fickian diffusion; and uniformity in nanoMIPs size have significant impact on release of drug. Swelling of nanoMIP is one of the dominant factors influencing the drug release patterns. The imprinting procedure and the studies reported in this study would be highly useful in future for cancer drug administration.


Assuntos
Antineoplásicos/farmacologia , Impressão Molecular/métodos , Nanoporos , Polímeros/química , Adsorção , Amigdalina/química , Amigdalina/farmacologia , Preparações de Ação Retardada , Difusão , Cinética , Microscopia de Força Atômica , Nanoporos/ultraestrutura , Propriedades de Superfície , Termogravimetria , Água/química
11.
Biosens Bioelectron ; 82: 20-5, 2016 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-27031187

RESUMO

Molecular imprints of the tobacco necrosis virus (TNV) have been formed within polythiophene nanofilms with an approximate thickness of 200nm. These films have been electrochemically deposited onto conducting Au surfaces. Upon rebinding, the TNV-polythiophene complex changes the fluorescence intensity of the nanofilm. The fluorescence intensity at 410nm was observed to be proportional to the concentration of viruses in the range of 0.1-10ngL(-1) (0.15-15pg) with the lower calculated detection limit of 2.29ngL(-1) (3.4pg). The intensity of the fluorescence emission is not affected by the thickness of the polythiophene film and the nature of TNV specific binding sites. Kinetic data analyses showed that the nanofilm responds to TNV within 2min; and cross-selectivity studies with tobacco mosaic virus (TMV) showed an excellent specificity for the targeted TNV. These binding experiments demonstrate the potential of fluorescence emission for the specific, label free and rapid detection of viruses using nanofilm sensors. Taking into account the lower limit of detection, the fluorescence sensing reported here is reliable, simple to perform, rapid, cost-effective and offers a sensitive analytical method for virus detection in water resources.


Assuntos
Água Potável/virologia , Impressão Molecular , Nanoestruturas/química , Polímeros/química , Tiofenos/química , Tombusviridae/isolamento & purificação , Fluorescência , Limite de Detecção , Espectrometria de Fluorescência/métodos , Nicotiana/virologia , Vírus do Mosaico do Tabaco/isolamento & purificação
12.
J Mol Recognit ; 28(7): 427-37, 2015 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-25703338

RESUMO

A new computational model capable of understanding the nature of interactions in signature complexes formed between the template (2,3,7,8-tetrachlorodibenzo-p dioxin (TCDD)) and the functional monomers (methacrylic acid (MAA)) using density functional theory (DFT) has been designed. The polymer precursors were optimized for geometries in polymerization media, computing the interaction energies between template molecules and functional monomers of transient pre-polymerized complexes (PPC), and structural and vibrational properties reference to theoretical infrared spectra were computed using DFT of B3LYP/6 311+G(d,p) hybrid functional method. Atom in molecule theory was used to analyze the hydrogen-bonding characteristics of PPC of MAA-TCDD. Considering the theoretical titrations conducted in a virtual solvent box, it was found that the 1:4 molar ratio was required to form the most stable PPC in a given solvent system. The electron density plots indicate strong hydrogen bonding as shown by the 2pz dominant highest occupied molecular orbital (HOMO) character that could be the preferable sites of binding for target molecule, TCDD. Considering HOMO approach, the active adsorption sites in molecularly imprinted polymer was modeled to get insight on molecular recognition property for targeted molecule, TCDD. The proposed computational protocol is simple, accurate, and novel to design the polymer and is useful to predict the properties of polymer systems than the conventional theoretical analysis of template-monomer interactions.


Assuntos
Simulação por Computador , Dioxinas/química , Nanoporos , Metacrilatos/química , Impressão Molecular
13.
Anal Bioanal Chem ; 406(22): 5313-21, 2014 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-24961636

RESUMO

Molecularly imprinted polymer (MIP) microspheres with diameters in the range 60-500 µm were synthesized in a continuous segmented flow microfluidic reactor and used as packing material for microtraps for the selective separation of benzo[a]pyrene (BAP) from environmental aqueous samples. The synthesis involved the pumping of monodisperse droplets of acetonitrile containing methacrylic acid as the functional monomer, BAP as a template, and ethylene glycol dimethacrylate as the cross-linking monomer into the microchannels of the microfluidic reactor. The microspheres showed high adsorption capacity and selectivity for BAP in aqueous solutions; both are important for the environmental monitoring and analysis of BAP. The adsorption capacity for BAP of the smallest MIP microspheres (size range 60-80 µm), prepared as part of this study, was 75 mg g(-1) in aqueous solutions; furthermore, this adsorption capacity was close to 300 % higher than that of commercially used activated carbon. Microtraps packed with MIP retained BAP intact for at least 30 days, whereas microtraps packed with activated carbon for BAP showed 40 % reduction in BAP concentration for the same period. This study has demonstrated that MIP microtraps have significant potential for the selective enrichment and preservation of targeted polycyclic aromatic hydrocarbons from complex environmental samples.


Assuntos
Monitoramento Ambiental/métodos , Microesferas , Hidrocarbonetos Policíclicos Aromáticos/química , Polímeros/química , Adsorção , Poluentes Atmosféricos/análise , Benzo(a)pireno/química , Meio Ambiente , Desenho de Equipamento , Teste de Materiais , Metacrilatos/química , Microfluídica , Impressão Molecular , Reprodutibilidade dos Testes , Águas Residuárias , Poluentes da Água/análise
14.
J Hazard Mater ; 274: 1-7, 2014 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-24759433

RESUMO

Im*plications due to oil spills on marine ecosystems have created a great interest toward developing more efficient and selective materials for oil spill toxins detection and remediation. This research paper highlights the application of highly efficient molecularly imprinted polymer (MIP) adsorbents based on a newly developed functional crosslinker (N,O-bismethacryloyl ethanolamine, NOBE) for detection of highly toxic polycyclic aromatic hydrocarbons (PAHs) in seawater. The binding capacity of MIP for oil spill toxin pyrene is 35 mg/g as compared to the value of 3.65 mg/g obtained using a non-imprinted polymer (NIP). The selectivity of all three high molecular weight PAHs (pyrene, chrysene and benzo[a]pyrene) on the NOBE-MIP shows an excellent selective binding with only 5.5% and 7% cross-reactivity for chrysene and benzo[a]pyrene, respectively. Not only is this particularly significant because the rebinding solvent is water, which is known to promote non-selective hydrophobic interactions; the binding remains comparable under salt-water conditions. These selective and high capacity adsorbents will find wide application in industrial and marine water monitoring/remediation.


Assuntos
Impressão Molecular , Hidrocarbonetos Policíclicos Aromáticos/análise , Polímeros/química , Poluentes Químicos da Água/análise , Adsorção , Reagentes de Ligações Cruzadas/química , Ecossistema , Monitoramento Ambiental , Etanolaminas/química , Metacrilatos/química , Poluição por Petróleo , Hidrocarbonetos Policíclicos Aromáticos/química , Água do Mar/análise , Poluentes Químicos da Água/química
15.
Environ Sci Pollut Res Int ; 21(10): 6603-11, 2014 May.
Artigo em Inglês | MEDLINE | ID: mdl-24499987

RESUMO

Molecularly imprinted polymer adsorbent has been prepared to remove a group of recalcitrant and acutely hazardous (p-type) chemicals from water and wastewaters. The polymer adsorbent exhibited twofold higher adsorption capacity than the commercially used polystyrene divinylbenzene resin (XAD) and powdered activated carbon adsorbents. Higher adsorption capacity of the polymer adsorbent was explained on the basis of high specific surface area formed during molecular imprinting process. Freundlich isotherms drawn showed that the adsorption of p-type chemicals onto polymer adsorbent was kinetically faster than the other reference adsorbents. Matrix effect on adsorption of p-type chemicals was minimal, and also polymer adsorbent was amenable to regeneration by washing with water/methanol (3:1, v/v) solution. The polymer adsorbent was unaltered in its adsorption capacity up to 10 cycles of adsorption and desorption, which will be more desirable in cost reduction of treatment compared with single-time-use activated carbon.


Assuntos
Preparações Farmacêuticas/análise , Polímeros/química , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Adsorção , Carvão Vegetal/química , Cinética , Impressão Molecular , Poliestirenos/química , Poluentes Químicos da Água/química
16.
Comb Chem High Throughput Screen ; 16(9): 682-94, 2013 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-24050695

RESUMO

Molecular imprinting is an interesting technique for preparation of molecular recognition materials with discriminating similar molecules from complex systems. In particular, imprinting more than one molecule has immense application in remediation of industrial waste. Major difficulty in molecular imprinting is the selection of suitable polymer precursors. In this article, authors have proposed a new computational approach for combinatorial screening of polymer precursor library to select appropriate polymer precursors to prepare imprinted polymer capable of selectively binding carcinogenic polycyclic aromatic hydrocarbons (PAHs). Molecular Dynamics (MD) and Quantum Mechanics (QM) models were used to compute interaction energy scores between polymer precursors and PAHs in a simulated solvent box. A self-designed virtual library of functional monomers has been prepared, and then used for MD simulations to screen the best functional monomers. Initially, molecules used in the study were geometrically optimized and then interaction energies were computed using density functional theory (DFT) in Becke 3-Parameter Exchange Correlation Function (B3LYP) level with 6-31G*basis set on Gaussian 4.1 Ver. software. Complimentary to theoretical predictions, selected polymers were prepared in laboratory and compared theoretically computed binding score with the binding capacity of the polymer on spectrofluorimetry. The computer simulations used in this research paper are rapid and reliable for the combinatorial screening of polymer precursors in experimental-free way to design of multi-template imprinted polymers.


Assuntos
Carcinógenos/química , Impressão Molecular/métodos , Hidrocarbonetos Policíclicos Aromáticos/química , Polímeros/química , Simulação por Computador , Modelos Moleculares , Teoria Quântica , Software
17.
J Mol Model ; 18(5): 1969-81, 2012 May.
Artigo em Inglês | MEDLINE | ID: mdl-21877152

RESUMO

A combinatorial screening procedure was used for the selection of polymer precursors in the preparation of molecularly imprinted polymer (MIP), which is useful in the detection of the air pollution marker molecule benzo[a]pyrene (BAP). Molecular imprinting is a technique for the preparation of polymer materials with specific molecular recognition receptors. The preparation of imprinted polymers requires polymer precursors such as functional monomer, cross-linking monomer, solvent, an initiator of polymerization and thermal or UV radiation. A virtual library of functional monomers was prepared based on interaction binding scores computed using HyperChem Release 8.0 software. Initially, the possible minimum energy conformation of the monomers and BAP were optimized using the semi-empirical (PM3) quantum method. The binding energy between the functional monomer and the template (BAP) was computed using the Hartree-Fock (HF) method with 6-31 G basis set, which is an ab initio approach based on Moller-Plesset second order perturbation theory (MP2). From the computations, methacrylic acid (MAA) and ethylene glycol dimethacrylate (EGDMA) were selected for preparation of BAP imprinted polymer. The larger interaction energy (ΔE) represents possibility of more affinity binding sites formation in the polymer, which provides high binding capacity. The theoretical predictions were complimented through adsorption experiments. There is a good agreement between experimental binding results and theoretical computations, which provides further evidence of the validity of the usefulness of computational screening procedures in the selection of appropriate MIP precursors in an experiment-free way.


Assuntos
Poluentes Ocupacionais do Ar/química , Benzo(a)pireno/química , Metacrilatos/química , Modelos Químicos , Polímeros/química , Adsorção , Sítios de Ligação , Técnicas de Química Combinatória , Simulação por Computador , Cinética , Bibliotecas Digitais , Impressão Molecular , Reprodutibilidade dos Testes , Termodinâmica , Raios Ultravioleta
18.
Environ Sci Pollut Res Int ; 19(5): 1841-51, 2012 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-22207238

RESUMO

INTRODUCTION: Microcystins (MCs; cyclic heptapeptides) are produced by freshwater cyanobacteria and cause public health concern in potable water supplies. There are more than 60 types of MCs identified to date, of which MC-LR is the most common found worldwide. For MC-LR, the WHO has established a threshold value of 1 µg L(-1) for drinking water. The present MCs removal methods such as coagulation, flocculation, adsorption, and filtration showed low efficiency for removing dissolved MC fraction from surface waters to the stipulated limit prescribed by WHO based on MC health impacts. The search for cost-effective and efficient removal method is still warranted for remediation of dissolved MC-LR-contaminated water resources. MATERIALS AND METHODS: Molecularly imprinted polymer (MIP) adsorbent has been prepared using non-covalent imprinting approach. Using MC-LR as a template, itaconic acid as a functional monomer, and ethylene glycol dimethacrylate as a cross-linking monomer, a MIP has been synthesized. Computer simulations were used to design effective binding sites for MC-LR binding in aqueous solutions. Batch binding adsorption assay was followed to determine binding capacity of MIP under the influence of environmental parameters such as total dissolved solids and pH. RESULTS AND DISCUSSION: The adsorptive removal of MC-LR from lake water has been investigated using MIPs. The MIP showed excellent adsorption potential toward MC-LR in aqueous solutions with a binding capacity of 3.64 µg mg(-1) which is about 60% and 70% more than the commercially used powdered activated carbon (PAC) and resin XAD, respectively. Environmental parameters such as total organic carbon (represented as chemical oxygen demand (COD)) and total dissolved solids (TDS) showed no significant interference up to 300 mg L(-1) for MC-LR removal from lake water samples. It was found that the binding sites on PAC and XAD have more affinity toward COD and TDS than the MC-LR. Further, the adsorption capacity of the MIP was evaluated rigorously by its repeated contact with fresh lake water, and it was found that the adsorption capacity of the MIP did not change even after seven adsorption/desorption cycles. The contaminated water of MC-LR (1.0 µg L(-1)) of 3,640 L could be treated by 1 g of MIP with an estimated cost of US $1.5. CONCLUSIONS: The adsorption capacity of the MIP is 40% more than commercially used PAC and resins and also the polymer showed reusable potential which is one of the important criteria in selection of cyanotoxins remediation methods.


Assuntos
Microcistinas/isolamento & purificação , Polímeros/química , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água/métodos , Adsorção , Análise da Demanda Biológica de Oxigênio , Água Doce , Lagos , Impressão Molecular , Polímeros/síntese química , Succinatos/química , Propriedades de Superfície
19.
Anal Bioanal Chem ; 397(7): 3097-106, 2010 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-20526768

RESUMO

A method based on solid--phase extraction with a molecularly imprinted polymer (MIP) has been developed to determine five probable human carcinogenic polycyclic aromatic hydrocarbons (PAHs) in ambient air dust by gas chromatography-mass spectrometry (GC-MS). Molecularly imprinted poly(vinylpyridine-co-ethylene glycol dimethacrylate) was chosen as solid-phase extraction (SPE) material for PAHs. The conditions affecting extraction efficiency, for example surface properties, concentration of PAHs, and equilibration times were evaluated and optimized. Under optimum conditions, pre-concentration factors for MIP-SPE ranged between 80 and 93 for 10 mL ambient air dust leachate. PAHs recoveries from MIP-SPE after extraction from air dust were between 85% and 97% and calibration graphs of the PAHs showed a good linearity between 10 and 1000 ng L(-1) (r = 0.99). The extraction efficiency of MIP for PAHs was compared with that of commercially available SPE materials--powdered activated carbon (PAC) and polystyrene-divinylbenzene resin (XAD)--and it was shown that the extraction capacity of the MIP was better than that of the other two SPE materials. Organic matter in air dust had no effect on MIP extraction, which produced a clean extract for GC-MS analysis. The detection limit of the method proposed in this article is 0.15 ng L(-1) for benzo[a]pyrene, which is a marker molecule of air pollution. The method has been applied to the determination of probable carcinogenic PAHs in air dust of industrial zones and satisfactory results were obtained.


Assuntos
Poluentes Atmosféricos/análise , Poeira/análise , Cromatografia Gasosa-Espectrometria de Massas/métodos , Hidrocarbonetos Policíclicos Aromáticos/análise , Hidrocarbonetos Policíclicos Aromáticos/isolamento & purificação , Polímeros/química , Extração em Fase Sólida/instrumentação , Adsorção , Limite de Detecção , Metacrilatos/química , Impressão Molecular , Polivinil/química , Extração em Fase Sólida/métodos
20.
Water Res ; 44(3): 681-8, 2010 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-19822345

RESUMO

A molecularly imprinted polymer (MIP) adsorbent for carcinogenic polycyclic aromatic hydrocarbons (PAHs) was prepared using a non-covalent templating technique. MIP particles sized from 2 to 5 microm were synthesized in acetonitrile by using six PAHs mix as a template, methacrylic acid as the functional monomer, and ethylene glycol dimethacrylate as the cross-linker. When compared with the non-imprinted polymer (NIP), the MIP showed an excellent affinity towards PAHs in aqueous solution with binding capacity (B(max)) of 687 microg g(-1)MIP, imprinting effect of 6, and a dissociation constant of 24 microM. The MIP exhibited significant binding affinity towards PAHs even in the presence of environmental parameters such as dissolved organic matter (COD) and total dissolved inorganic solids (TDS), suggesting that this material may be appropriate for removal of carcinogenic PAHs. The feasibility of removing PAHs from water by the MIP demonstrated using groundwater spiked with PAHs. In addition, the MIP reusability without any deterioration in performance was demonstrated at least ten repeated cycles.


Assuntos
Carcinógenos/isolamento & purificação , Impressão Molecular/métodos , Hidrocarbonetos Policíclicos Aromáticos/isolamento & purificação , Polímeros/química , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água/métodos , Adsorção , Conservação dos Recursos Naturais , Meio Ambiente , Humanos , Microscopia Eletrônica de Varredura , Impressão Molecular/economia , Solo/análise , Propriedades de Superfície , Temperatura , Fatores de Tempo , Abastecimento de Água/análise
SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA
...