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1.
J Hazard Mater ; 384: 121254, 2020 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-31586911

RESUMO

Ethidium bromide (EtBr) is an intercalating agent commonly used as nucleic acid fluorescent tag in various techniques of life science field. It is considered as a serious biohazard due to its mutagenicity and carcinogenicity. As such, developing high efficiency and low cost materials as cleanup kits is in urgent need although many methods have already been developed. In this study we take use of the affinity of organic cations for clay minerals of high cation exchange capacity (CEC) and large specific surface area (SSA) and tested the removal of EtBr using rectorite, a type of clay mineral made of 1:1 regularly mixed layers of illite and montmorillonite. Our results showed that the uptake of Et+ on rectorite could be as high as 400 mmol/kg and the removal of Et+ was extremely fast. Desorption of inorganic cation Ca2+ and sorption of counterion Br- revealed that cation exchange was the dominating mechanism of Et+ removal using rectorite. Thermal analyses revealed that the EtBr could be thermally destructed inside the interlayer of rectorite and the material could be thermally regenerated. Thus, clay minerals could have a great potential to be fabricated into cleanup kits for the removal of EtBr in case of spill.

2.
Materials (Basel) ; 12(18)2019 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-31491854

RESUMO

The adsorption of atenolol (AT) from aqueous solutions by Ca-montmorillonite (SAz-2) was investigated in batch studies under different physicochemical conditions. The AT existed in neutral un-dissociated form at pH 10, and was adsorbed on dioctahedral smectite (SAz-2) obeying the Langmuir isotherm with a maximum adsorption capacity of 330 mmol/kg. The kinetic adsorption suggested that both strong and weak adsorption sites existed on SAz-2 and participated in the adsorption mechanisms. The amount of exchangeable cations desorbed from SAz-2 during AT adsorption was linearly correlated with the amounts of adsorbed AT having slopes of 0.43, which implied that a cation exchange based adsorption mechanism was also in place. A comprehensive basal spacing change of SAz-2 was observed after AT adsorption on the clay mineral when tested with or without AT recrystallization. The intercalation of AT into the SAz-2 interlayers did not result in swelling due to the low adsorption capacity of the drug. Prominent interactions between the pharmaceutical molecule and SAz-2 were evidenced by apparent shifts of the infrared absorption bands after adsorption. The interlayer configurations and hydrogen bonding of AT on SAz-2 were also supported by infrared, X-ray diffraction and thermogravimetric analyses. This study suggested that SAz-2 is an excellent material to remove not only AT from pharmaceutical wastewater, but can potentially remove many other ß-receptor blocker drugs. The results helped us to understand the possible interlayer configurations and adsorption mechanisms of the drugs on natural clay mineral based adsorbents.

3.
Sci Total Environ ; 669: 527-539, 2019 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-30884274

RESUMO

We investigated the subsurface biomatrix of the most abundant As-mineral, arsenopyrite (FeAsS), and meticulously studied a potential biogenic arsenic mobilization phenomenon. An arsenic-resistant [up to 7.5 mM As(III) and 200 mM As(V)] and arsenate-reducing bacterial strain (Staphylococcus sp. As-3) was isolated from a sediment core sample taken from the Budai borehole, on the southwestern coast of Taiwan. Isolate As-3 could reduce 5 mM As(V) to 3.04 mM in 96 h, generating 1.6 mM As(III) under anoxic conditions. Isolate As-3, which adsorbed As(V) up to 19.02 mg g-1 (cdw) and As(III) up to 0.46 mg g-1 (cdw), demonstrated effective As-bioaccumulating ability, as corroborated by a TEM-EDS analysis. Under anaerobic batch conditions, isolate As-3 micro-colonies could grow on as well as interact with arsenopyrite (FeAsS), mobilizing arsenic into soluble phase as As(III) and As(V). Using synchrotron radiation-based FTIR micro-spectroscopy, various functional group signatures and critical chemical bonds enabling a direct interaction with arsenopyrite were underpinned, such as a potential P-OFe bond involved in facilitating bacteria-mineral interaction. Using atomic force microscopy, we analyzed the scattered bacterial cell arrangement and structure and measured various biomechanical properties of micro-colonized Staphylococcus sp. As-3 cells on arsenopyrite. We suggest that the release of organic acids from As-3 drives soluble arsenic release in the aqueous phase under anoxic conditions through oxidative dissolution. Furthermore, arsC-encoding putative cytoplasmic arsenic reductase sequencing and transcript characterization indicated that arsC plays a possible role in the reduction of moderately soluble As(V) to highly soluble toxic As(III) under anoxic conditions. Thus, we suggest that firmicutes such as Staphylococcus sp. As-3 may play an important role in microbially-mediated arsenic mobilization, leading to arsenic release in the sub-surface niche.


Assuntos
Arsênio/toxicidade , Poluentes do Solo/toxicidade , Staphylococcus/fisiologia , Adaptação Fisiológica , Arsênio/análise , Arsenicais , Monitoramento Ambiental , Sedimentos Geológicos/química , Sedimentos Geológicos/microbiologia , Compostos de Ferro , Minerais , Poluentes do Solo/análise , Sulfetos , Taiwan
4.
J Hazard Mater ; 373: 187-196, 2019 07 05.
Artigo em Inglês | MEDLINE | ID: mdl-30921569

RESUMO

Uptake of metals, organics, and formation of metal-organic complexes on the surface or in the interlayer of clay minerals had been studied extensively over the last half century. In this study, we investigated the uptake mechanisms of Cu2+, triethylenetetramine (TETA), and Cu-TETA on rectorite and its use for metal removal via metal-TETA complexation. The uptake of Cu2+, TETA, and Cu-TETA by rectorite occurred on the external as well as in the interlayer space, resulting in a change of d001-spacing due to differences in sizes of interlayer cations or complexes. Although the uptake of Cu2+ and Cu-TETA by rectorite was via a cation exchange process as evidenced by the stoichiometric desorption of dominant interlayer cation Ca2+, the uptake of TETA alone on rectorite was via complexation with interlayer cation Ca2+. Due to strong affinity of TETA for Cu2+, significant amounts of Cu2+ uptake occurred on TETA-rectorite. Desorption of Ca2+ from TETA-rectorite confirmed the replacement of interlayer cation Ca2+ by Cu2+. However, the replacement of Ca2+ by Cu2+ in TETA-rectorite did not involved in removal of TETA. As such, TETA-modified clay minerals may serve as a type of sorbents for the removal of selected heavy metals via surface or interlayer via complexation.

5.
J Hazard Mater ; 368: 487-495, 2019 04 15.
Artigo em Inglês | MEDLINE | ID: mdl-30710777

RESUMO

Calcined hydrotalcite (CHT) was evaluated for its potential removal of perfluorooctanoic acid (PFOA) from water in this study. The uptake of PFOA by CHT could be as high as 1587 mg/g (ca. 3.8 mmol/g), slightly larger than the anion exchange capacity (AEC) of the hydrotalcite (HT). Such a high removal was fast and pH independent, suggesting the versatile use of CHT. Due to the structural memory effect of HT, the removal involved adsorption of PFOA during HT recovery and intercalation of PFOA into the interlayer of restructured HT at low and high initial concentrations, respectively. Limited by the specific surface area and AEC, the intercalated PFOA would form a vertical bilayer or admicelle conformation. As such, the HT intercalated with PFOA became one-layer stacking with a basal spacing of 2.04 nm in contrast to the 3R polytype of recovered HT having a layer thickness of 0.78 nm, as confirmed by X-ray diffraction, thermogravimetric, and infra-red analyses. Due to its high PFOA removal capacity and large partitioning coefficient, the amount of CHT used, thus, the disposal of PFOA-laden solid could be minimized.

6.
J Hazard Mater ; 364: 671-681, 2019 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-30399550

RESUMO

A gram-positive spore former, Lysinibacillus sp. B2A1 was isolated from a high arsenic containing groundwater of Beimen2A well, Chianan Plain area, Southwestern Taiwan. Noteworthy, in the subsurface-mimicking anoxic incubation with a Na-lactate amendment system, this isolate could interact with arsenic-source mineral arsenopyrite and enhance arsenic mobilization. Further, the isolate showed elevated levels of arsenic resistance, 200 mM and 7.5 mM for arsenate and arsenite, respectively. Lysinibacillus sp. B2A1 demonstrated condition-specific redox activities including salient oxic oxidation of arsenite and anoxic reduction of arsenate. The elevated rate of As(III) oxidation (Vmax = 0.13 µM min-1 per 106 cells, Km = 15.3 µM) under oxic conditions was potent. Correlating with stout persistence in an arsenic-rich niche, remarkably, the lesser toxic effects of arsenic ions on bacterial sporulation frequency and germination highlight this strain's ability to thrive under catastrophic conditions. Moreover, the whole genome analysis elucidated diverse metal redox/resistance genes that included a potential arsenite S-adenosylmethyltransferase capable of mitigating arsenite toxicity. Owing to its arsenic resistance, conditional redox activities and ability to interact with arsenic minerals leading to arsenic mobilization, the presence of such spore-forming strains could be a decisive indication towards arsenic mobilization in subsurface aquifers having a high concentration of soluble arsenic or its source minerals.


Assuntos
Arsênio/metabolismo , Arsenicais/metabolismo , Bacillaceae/genética , Genoma Bacteriano , Compostos de Ferro/metabolismo , Minerais/metabolismo , Sulfetos/metabolismo , Bacillaceae/metabolismo , Bacillaceae/fisiologia , Genes Bacterianos , Água Subterrânea/microbiologia , Oxirredução , Esporos Bacterianos , Microbiologia da Água
7.
Sci Total Environ ; 642: 198-207, 2018 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-29898425

RESUMO

Tyramine (TY) adsorption on a Ca-montmorillonite (SAz-2) was investigated with batch experiments and complementary analyses utilizing ultra-high performance liquid chromatography, ion chromatography, X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, and thermogravimetry (TG). The adsorption reached equilibrium in 8 h, complying with the pseudo-second-order rate equation, and came to an adsorption capacity of 682 mmol kg-1 at pH 6-8.1, utilizing the Langmuir isotherm model. The adsorption of TY and desorption of exchangeable cations exhibited a linear relationship with a slope of 0.9, implying that the adsorption was largely influenced by a cation exchange mechanism. The effective adsorption was further verified by the characteristic TY bands in the FTIR spectra and the signals of mass loss due to TY decomposition in the TG measurements of the clay after adsorption experiments. Intercalation of hydrated TY into the clay interlayer was confirmed by XRD and TG analyses of the heated samples loaded with TY. The adsorption reached only 0.57 cation exchange capacity of the clay which was probably limited by the low charge density of TY as compared to the negative charge density of the clay surface and by the steric effects arising from the hydration of TY that increased its molecular size. Adsorption of TY on montmorillonite can make TY more resistant to thermal decomposition and possibly better preserved in aquatic and soil environments.

8.
Sci Rep ; 6: 37400, 2016 11 17.
Artigo em Inglês | MEDLINE | ID: mdl-27853275

RESUMO

The frequencies of microwave absorption can be affected by the permanent electric dipole moment which could be adjusted by modifying the crystal symmetry of the microwave absorbing materials. Herein, we corroborate this strategy experimentally and computationally to the microwave absorption of manganese dioxides. Nanosized Co-doped cryptomelane (Co-Cryp) was successfully synthesized by a one-step reaction. The introduction of Co(III) induced a change of crystal symmetry from tetragonal to monlclinic, which could lead to an increase of its permanent electric dipole moment. As a result, the frequencies of maximum microwave absorption were regulated in the range of 7.4 to 13.9 GHz with a broadened bandwidths. The results suggested that microwave absorption of manganese dioxides can be tailored with Co doping to expand their potential uses for abatement of various microwave pollutions.

9.
J Nanosci Nanotechnol ; 16(4): 3835-40, 2016 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-27451720

RESUMO

The aim of this study was to explore a new nano-composite carbon adsorbent material for the removal of arsenic from water. The multilayer carbon nanotubes (MCNTs) were treated with different acids and/or modified with iron to create more surface COOH sites or Fe-impregnated MCNTs for the enhanced uptake of As(V). Tests were conducted as a function of initial As(V) concentrations, contact time, and solution pH. The coverage of ferric hydroxides on MCNTs and the uptake of As on Fe-MCNTs were independently confirmed by field emission scanning electron microscope and energy dispersive X-ray spectroscopy analyses. With an As(V) uptake capacities of 27 mg/g on Fe-MCNTs and 14 mg/g on acid-MCNTs, the material showed superior performance for As(V) removal.

10.
Sci Total Environ ; 569-570: 212-222, 2016 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-27343940

RESUMO

High arsenic abundance of 50-700µg/L in the groundwater from the Chianan Plain in southwestern Taiwan is a well-known environmental hazard. The groundwater-associated sediments, however, have not been geochemically characterized, thus hindering a comprehensive understanding of arsenic cycling in this region. In this study, samples collected from a 250m sediment core at the centre of the Chianan Plain were analyzed for arsenic and TOC concentrations (N=158), constituent minerals (N=25), major element abundances (N=105), and sequential arsenic extraction (N=23). The arsenic data show a prevalence of >10mg/kg with higher concentrations of 20-50mg/kg concentrated at 60-80 and 195-210m. Arsenic was extracted mainly as an adsorbate on clay minerals, as a co-precipitate in amorphous iron oxyhydroxide, and as a structural component in clay minerals. Since the sediments consist mainly of quartz, chlorite, and illite, the correlations between arsenic concentration and abundances of K2O and MgO pinpoint illite and chlorite as the major arsenic hosts. The arsenic-total iron correlation reflects the role of chlorite along with the contribution from amorphous iron oxyhydroxide as indicated by arsenic extraction data. Organic matter is not the dominant arsenic host for low TOC content, low arsenic abundance extracted from it, and a relatively low R(2) of the arsenic-TOC correlation. The major constituent minerals in the sediments are the same as those of the upriver metapelites, establishing a sink-source relationship. Composition data from two deep groundwater samples near the sediment core show Eh values and As(V)/As(III) ratios of reducing environments and high arsenic, K, Mg, and Fe contents necessary for deriving arsenic from sediments by desorption from clay and dissolution of iron oxyhydroxide. Therefore, groundwater arsenic was mainly derived from groundwater-associated sediments with limited contributions from other sources, such as mud volcanoes.


Assuntos
Arsênio/análise , Carbono/análise , Sedimentos Geológicos/análise , Poluentes Químicos da Água/análise , Monitoramento Ambiental , Água Subterrânea/química , Rios/química , Taiwan
11.
Chemosphere ; 155: 292-299, 2016 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-27131449

RESUMO

With the increased detections of commonly used pharmaceuticals in surface water and wastewater, extensive attentions were paid recently to the fate and transport of these pharmaceuticals in the environment. Amitriptyline (AMI) is a tricyclic antidepressant widely applied to treat patients with anxiety and depression. In this study, the removal of AMI with palygorskite clay (PFl-1) was investigated under different physico-chemical conditions and supplemented by instrumental analyses. The uptake of AMI on PFl-1 was well fitted by the Langmuir isotherm with an adsorption capacity of 0.168 mmol g(-1) at pH 6-7. The AMI uptake was fast and reached equilibrium in 15 min. The X-ray diffraction patterns showed no shift of the (110) peak position of palygorskite after AMI uptake. However, the (001) peak position of the minor component smectite (about 10%) shifted to lower angle as the amounts of AMI input increased. These results suggested surface uptake of AMI on palygorskite and interlayer uptake of AMI in smectite. As smectite is a common component of palygorskite clays, its role in assessing the properties and performances of palygorskite clays for the uptake and removal of contaminants should not be neglected. Overall, the high affinity of AMI for PFl-1 and strong retention of AMI on PFl-1 suggested that it could be a good adsorbent to remove AMI from wastewater. Palygorskite clays can also be a sink for many cationic pharmaceuticals in the environmental of the arid regions.


Assuntos
Silicatos de Alumínio/química , Amitriptilina/química , Poluentes Químicos da Água/química , Adsorção , Amitriptilina/análise , Cátions , Argila , Concentração de Íons de Hidrogênio , Compostos de Magnésio/química , Silicatos/química , Compostos de Silício/química , Águas Residuárias , Água/química , Poluentes Químicos da Água/análise , Difração de Raios X
12.
Colloids Surf B Biointerfaces ; 140: 67-73, 2016 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-26735896

RESUMO

As natural ingredients and excipients, kaolinite and talc were frequently studied for their interactions with drugs in pharmaceutical formulations. In this study, the uptake of ranitidine (RT) on these two minerals was studied under different physic-chemical conditions and the mechanism of RT uptake on these two minerals contrasted. Although the thermodynamic and kinetic RT uptake on these two minerals was similar and the RT uptake on both minerals were limited to the external surfaces only, drastic difference in RT uptake was found under different equilibrium solution pH and ionic strength conditions. As cation exchange process was strongly affected by solution pH and ionic strength, the RT uptake on kaolinite was dominated by cation exchange and electrostatic interactions, while the RT uptake on talc was more controlled by inter- and intra- molecular hydrogen bonding interactions. For kaolinite, the limiting factor for RT uptake was the specific surface area due to monolayer RT adsorption. In contract, multilayer RT uptake was found on talc surfaces. No matter which mechanism dominated RT uptake on these minerals, the interaction should not be neglected in pharmaceutical formulations should these minerals be used as additives and/or excipients.


Assuntos
Excipientes/química , Caulim/química , Ranitidina/química , Talco/química , Adsorção , Algoritmos , Ligação de Hidrogênio , Concentração de Íons de Hidrogênio , Cinética , Modelos Químicos , Estrutura Molecular , Concentração Osmolar , Eletricidade Estática , Termodinâmica
13.
J Hazard Mater ; 303: 55-63, 2016 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-26513564

RESUMO

The adsorption of ciprofloxacin (CIP) as well as probe compounds, phenylpiperazine (PP) (NH) and fluorochloroquinolone carboxylic acid (FCQCA) (COOH), on palygorskite (PFl-1) obeyed the Langmuir isotherm at pH 2, 7, and 11 except the FCQCA adsorption at pH 2. The CIP and PP adsorption onto PFl-1 was 98-160 mmol/kg. In neutral solution the total amount of exchangeable cations desorbed correlated with the adsorbed amount of CIP and PP well with a slope of 0.9-1, indicating a cation-exchange mechanism. A low amount of FCQCA adsorption of 27-57 mmol/kg was observed and the amount of exchangeable cations desorbed negatively correlate with the amount of FCQCA adsorbed as influenced by surface complexation or cation bridging. FTIR band shifting due to the ring-stretch vibration of PP and the keto-carbonyl group stretching of FCQCA suggested strong interactions as PP and FCQCA absorbed on PFl-1 in neutral solution. In the interaction of CIP with PFl-1, the piperazine-amine group played an important role in cation-exchange interaction in acidic to neutral solution, while the deprotonated keto carbonyl group actively partook in cation bridging or surface complexation with metal cations adsorbed on PFl-1 when the CIP was in anionic form in alkaline solution.


Assuntos
Antibacterianos/química , Ciprofloxacina/química , Compostos de Magnésio/química , Compostos de Silício/química , Adsorção , Concentração de Íons de Hidrogênio , Troca Iônica , Espectroscopia de Infravermelho com Transformada de Fourier , Termodinâmica , Difração de Raios X
14.
J Hazard Mater ; 270: 169-75, 2014 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-24572273

RESUMO

Ionic liquids (ILs), due to their low vapor pressure, have been explored as green solvents for organic synthesis. In this study, the uptake of ILs on a high charge Ca-montmorillonite (MMT) and the use of the IL-modified MMT for the removal of anionic contaminants from water were systematically studied. Uptake of ILs by MMT was exclusively resulted from a cation exchange mechanism when the initial IL concentrations were less than the critical micelle concentration (CMC) and the sorbed ILs formed a monolayer conformation on the surface of MMT. When the initial IL concentrations were greater than the CMC, both cation exchange and hydrophobic interactions were responsible for the IL uptake. The IL molecules formed admicelles and the surface charge was reversed to positive balanced by counterion Cl(-) when the IL loading was higher than the cation exchange capacity of the mineral. The modified MMT could remove chromate from water instantaneously, with an adsorption capacity of 190 mmol/kg and a 99.5% removal efficiency at an initial chromate concentration of 2.6 mmol/L. These features could further expand the application of ILs and enable IL-modified MMT to be used as inexpensive sorbents for the removal of chromate and other oxyanions from water.


Assuntos
Bentonita/química , Cromatos/química , Líquidos Iônicos/química , Compostos de Potássio/química , Poluentes Químicos da Água/química , Adsorção , Troca Iônica , Propriedades de Superfície , Purificação da Água/métodos
15.
J Hazard Mater ; 277: 44-52, 2014 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-24373983

RESUMO

The uptake of amitriptyline (AMI) from aqueous environment by Ca-montmorillonite (SAz-2) was studied in a batch system under different physicochemical conditions. The adsorbent was characterized by X-ray diffraction and Fourier transform infrared (FTIR) analyses. The AMI adsorption on SAz-2 obeyed the Langmuir isotherm with a capacity of 330mg/g (1.05mmol/g) at pH 6-7. The adsorption kinetics was fast, almost reaching equilibrium in 2h, and followed a pseudo-second-order kinetic model. Desorption of exchangeable cations correlated with the AMI adsorption well, indicating that cation exchange was the major mechanism. X-ray diffraction patterns showing significant expansions of the d001 spacing and characteristic FTIR band shifts toward higher frequencies after AMI adsorption onto SAz-2 indicated that the adsorbed AMI molecules were intercalated into the interlayers of the mineral. Thermodynamic parameters based on partitioning coefficients suggested that the AMI adsorption was an endothermic physisorption at high adsorption levels. At low and higher AMI adsorption levels, the intercalated AMI molecules take a horizontal monolayer and bilayer conformation, respectively. The higher adsorption capacity suggested that SAz-2 could be a good candidate to remove AMI from wastewater and would be an important environmental sink for the fate and transport of AMI in soils and groundwater.


Assuntos
Amitriptilina/química , Bentonita/química , Cálcio/química , Poluentes do Solo/química , Poluentes Químicos da Água/química , Purificação da Água/métodos , Adsorção , Amitriptilina/isolamento & purificação , Cátions , Cinética , Modelos Químicos , Modelos Moleculares , Estrutura Molecular , Poluentes do Solo/isolamento & purificação , Espectroscopia de Infravermelho com Transformada de Fourier , Propriedades de Superfície , Poluentes Químicos da Água/isolamento & purificação
16.
J Colloid Interface Sci ; 411: 198-203, 2013 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-24041550

RESUMO

As the most commonly prescribed tricyclic antidepressant, amitriptyline (AT) is frequently detected in wastewater, surface runoff, and effluents from sewage treatment plants, and could potentially reach agriculture land through the application of municipal biosolids or reclaimed water. Kaolinite is one of the most important soil components under warm and humid climate conditions. In this study, the uptake and retention of AT by kaolinite from aqueous solution were investigated by batch tests, XRD, and FTIR analyses. The uptake of AT on kaolinite was instantaneous, attributed to surface adsorption as confirmed by XRD analyses. Quantitative correlation between desorption of exchangeable cations and AT adsorption confirmed experimentally that cation exchange was the dominant mechanism of AT uptake on kaolinite. The values for free energy of adsorption also suggested physi-sorption such as cation exchange. Solution pH had minimal influence at pH 5-11 even though the pKa value of AT was 9.4 and the surface charge of kaolinite was pH-dependent.


Assuntos
Amitriptilina/química , Caulim/química , Adsorção , Concentração de Íons de Hidrogênio , Cinética , Concentração Osmolar , Soluções , Espectroscopia de Infravermelho com Transformada de Fourier , Temperatura , Difração de Raios X
17.
J Hazard Mater ; 250-251: 362-9, 2013 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-23474410

RESUMO

With more pharmaceuticals and personal care products detected in the surface and waste waters, studies on interactions between these contaminants and soils or sediments have attracted great attention. In this study, the removal of ciprofloxacin (CIP), a fluoroquinolone antibiotic, by birnessite, a layered manganese oxide, in aqueous solution was investigated by batch studies supplemented by X-ray diffraction (XRD) and Fourier transform infrared analyses. Stoichiometric release of exchangeable cations accompanying CIP removal from water confirmed cation exchange as the major mechanism for CIP uptake by birnessite. Interlayer expansion after CIP adsorption on birnessite as revealed by XRD analyses indicated that intercalation contributed significantly to CIP uptake in addition to external surface adsorption. Correlation of CIP adsorption to specific surface area and cation exchange capacity suggested that the former was the limiting factor for CIP uptake. At the adsorption maximum, CIP molecules formed a monolayer on the birnessite surfaces. The adsorbed CIP could be partially removed using a cationic surfactant at a low initial concentration and mostly removed by AlCl3 at a higher initial concentration, which further supported the cation exchange mechanism for CIP removal by birnessite. The results indicated that the presence of layered Mn-oxide in the soil and waste water treatment systems may provide host for CIP accumulation.


Assuntos
Anti-Infecciosos/isolamento & purificação , Ciprofloxacina/isolamento & purificação , Óxidos/química , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água/métodos , Adsorção , Antibacterianos/farmacologia , Anti-Infecciosos/análise , Calibragem , Cátions , Cetrimônio , Compostos de Cetrimônio/química , Ciprofloxacina/análise , Fluoroquinolonas/química , Concentração de Íons de Hidrogênio , Compostos de Manganês/química , Espectrofotometria , Espectroscopia de Infravermelho com Transformada de Fourier , Propriedades de Superfície , Tensoativos , Água/química , Poluentes Químicos da Água/análise , Difração de Raios X
18.
Water Res ; 47(1): 259-68, 2013 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-23123088

RESUMO

Desorption from soil clay components may affect the transport and fate of antibiotics in the environment. In this study, ciprofloxacin (CIP) desorption from a kaolinite and a montmorillonite was investigated under different pHs, different concentrations of metal cations of various valencies (Na(+), Ca(2+) and Al(3+)) and a cationic surfactant hexadecyltrimethylammonium (HDTMA), and different desorption cycles. Desorption of CIP from kaolinite and montmorillonite was strongly pH-dependent and desorption isotherms were well fitted with the Langmuir equation. The percentage of CIP desorbed increased with increasing initial CIP loadings, desorbing cation concentrations, and desorption cycles. Comparatively, CIP was more readily desorbed from kaolinite than from montmorillonite. Moreover, the hysteresis index values were all negative, suggesting that the presence of metal cations and HDTMA in solution promoted CIP desorption from clay minerals, owing to cation exchange. The XRD analyses indicated that desorption of CIP occurred from both external and interlayer surfaces of montmorillonite. Formation of Al-CIP complex on solid surface and then detachment of Al-CIP from the solid surface may contribute to the higher CIP desorption by Al(3+) in comparison to Na(+) and Ca(2+).


Assuntos
Silicatos de Alumínio/química , Antibacterianos/química , Ciprofloxacina/química , Adsorção , Alumínio , Bentonita/química , Cálcio , Argila , Caulim/química , Cinética , Estrutura Molecular , Sódio , Espectroscopia de Infravermelho com Transformada de Fourier , Propriedades de Superfície , Poluentes Químicos da Água/química
19.
J Hazard Mater ; 221-222: 118-23, 2012 Jun 30.
Artigo em Inglês | MEDLINE | ID: mdl-22542779

RESUMO

Cr(VI) is a group A chemical based on the weight of evidence of carcinogenicity. Its transport and retention in soils and groundwater have been studied extensively. Zeolite is a major component in deposits originated from volcanic ash and tuff after alteration. In this study, zeolite aggregates with the particle size of 1.4-2.4mm were preloaded with Fe(III). The influence of present Fe(III) on Cr(VI) retention by and transport through zeolite was studied under batch and column experiments. The added Fe(III) resulted in an enhanced Cr(VI) retention by the zeolite with a capacity of 82mg/kg. The Cr(VI) adsorption on Fe(III)-zeolite followed a pseudo-second order kinetically and the Freundlich adsorption isotherm thermodynamically. Fitting the column experimental data to HYDRUS-1D resulted in a retardation factor of 3 in comparison to 5 calculated from batch tests at an initial Cr(VI) concentration of 3mg/L. The results from this study showed that enhanced adsorption and retention of Cr(VI) may happen in soils derived from volcanic ash and tuff that contains significant amounts of zeolite with extensive Fe(III) coating.


Assuntos
Cromo/química , Compostos Férricos/química , Zeolitas/química , Adsorção , Concentração de Íons de Hidrogênio , Cinética , Microscopia Eletrônica de Varredura , Concentração Osmolar , Temperatura
20.
J Colloid Interface Sci ; 360(1): 227-32, 2011 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-21570085

RESUMO

Frequent detection of pharmaceuticals in surface water and wastewater attracted renewed attention on studying interactions between pharmaceuticals and sludge or biosolids generated from wastewater treatment. Less attention was focused on studying interactions between pharmaceuticals and clay minerals, important soil and sediment components. This research targeted on investigating interactions between diphenhydramine (DPH), an important antihistamine drug, and a montmorillonite, a swelling clay, in aqueous solution. Stoichiometric desorption of exchangeable cations accompanying DPH adsorption confirmed that cation exchange was the most important mechanism of DPH uptake by the swelling clay. When the solution pH was below the pK(a) of DPH, its adsorption on the swelling clay was less affected by pH. Increasing solution pH above the pK(a) value resulted in a decrease in DPH adsorption by the clay. An increase in d(001) spacing at a high DPH loading level suggested interlayer adsorption, thus, intercalation of DPH. The results from this study showed that swelling clays are a good environmental sink for weak acidic drugs like DPH. In addition, the large cation exchange capacity and surface area make the clay a good candidate to remove cationic pharmaceuticals from the effluent of wastewater treatment facilities.


Assuntos
Bentonita/química , Difenidramina/isolamento & purificação , Poluentes Químicos da Água/química , Adsorção , Concentração de Íons de Hidrogênio , Propriedades de Superfície
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