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1.
Spectrochim Acta A Mol Biomol Spectrosc ; 316: 124340, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-38676986

RESUMO

Three CPs [Zn2(PDA)2(BMIOPE)2·3H2O]n (1), [Co(Br-BDC)(BMIOPE)]n (2) and [Co(MIP)(BMIOPE)]n (3) were synthesized by solvothermal method based on dual-ligand strategy (H2PDA, Br-H2BDC, BMIOPE and H2MIP are 1,3-phenylenediacetic acid, 5-bromo-isophthalic acid, 4,4'-bis(2-methylimidazol-1-yl)diphenyl ether and 5-methylisophthalic acid, respectively). Complexes 1 and 3 exhibit twofold parallel interwoven sql nets. Complex 2 is 2D layer structure. The luminescence property investigations showed that complexes 1-3 could act as multi-responsive fluorescent sensors to detect UO22+, Cr2O72- and CrO42- and nitrofurantoin (NFT) through fluorescence turn-off process, presenting excellent sensitivity and selectivity. Finally, the possible fluorescent quenching mechanisms of complexes 1-3 toward the above pollutants are also further investigated by employing spectroscopic methods and quantum chemical calculations. The fluorescence lifetime measurements manifest the mechanism of fluorescence quenching is static quenching process.

2.
Environ Sci Technol ; 58(8): 3974-3984, 2024 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-38306233

RESUMO

In contaminated water and soil, little is known about the role and mechanism of the biometabolic molecule siderophore desferrioxamine-B (DFO) in the biogeochemical cycle of uranium due to complicated coordination and reaction networks. Here, a joint experimental and quantum chemical investigation is carried out to probe the biomineralization of uranyl (UO22+, referred to as U(VI) hereafter) induced by Shewanella putrefaciens (abbreviated as S. putrefaciens) in the presence of DFO and Fe3+ ion. The results show that the production of mineralized solids {hydrogen-uranium mica [H2(UO2)2(PO4)2·8H2O]} via S. putrefaciens binding with UO22+ is inhibited by DFO, which can both chelate preferentially UO22+ to form a U(VI)-DFO complex in solution and seize it from U(VI)-biominerals upon solvation. However, with Fe3+ ion introduced, the strong specificity of DFO binding with Fe3+ causes re-emergence of biomineralization of UO22+ {bassetite [Fe(UO2)2(PO4)2·8(H2O)]} by S. putrefaciens, owing to competitive complexation between Fe3+ and UO22+ for DFO. As DFO possesses three hydroxamic functional groups, it forms hexadentate coordination with Fe3+ and UO22+ ions via these functional groups. The stability of the Fe3+-DFO complex is much higher than that of U(VI)-DFO, resulting in some DFO-released UO22+ to be remobilized by S. putrefaciens. Our finding not only adds to the understanding of the fate of toxic U(VI)-containing substances in the environment and biogeochemical cycles in the future but also suggests the promising potential of utilizing functionalized DFO ligands for uranium processing.


Assuntos
Shewanella putrefaciens , Urânio , Biomineralização , Desferroxamina/metabolismo , Desferroxamina/farmacologia , Shewanella putrefaciens/metabolismo , Sideróforos/metabolismo , Sideróforos/farmacologia , Urânio/química , Compostos de Ferro/química
3.
Small ; 20(23): e2308910, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38150628

RESUMO

The efficient removal of radioactive uranium from aqueous solution is of great significance for the safe and sustainable development of nuclear power. An ultrathin 2D metal-organic framework (MOF) nanosheet with cavity structures was elaborately fabricated based on a calix[4]arene ligand. Incorporating the permanent cavity structures on MOF nanosheet can fully utilize its structural characteristics of largely exposed surface area and accessible adsorption sites in pollutant removal, achieving ultrafast adsorption kinetics, and the functionalized cavity structure would endow the MOF nanosheets with the ability to achieve preconcentration and extraction of uranium from aqueous solution, affording ultrahigh removal efficiency even in ultra-low concentrations. Thus, more than 97% uranium can be removed from the concentration range of 50-500 µg L-1 within 5 min. Moreover, the 2D nano-material exhibits ultra-high anti-interference ability, which can efficiently remove uranium from groundwater and seawater. The adsorption mechanism was investigated by X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR) analysis, and density functional theory (DFT) calculations, which revealed that the cavity structure plays an important role in uranium capture. This study not only realizes highly efficient uranium removal from aqueous solution but also opens the door to achieving ultrathin MOF nanosheets with cavity structures, which will greatly expand the applications of MOF nanosheets.

4.
Molecules ; 28(12)2023 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-37375227

RESUMO

A new Ni coordination polymer [Ni(MIP)(BMIOPE)]n (1) was constructed (BMIOPE = 4,4'-bis(2-methylimidazol-1-yl)diphenyl ether, and H2MIP = 5-methylisophthalic acid), possessing two-dimensional (2D) twofold parallel interwoven net structure with a 44∙62 point symbol. Complex 1 has been successfully obtained based on mixed-ligand strategy. The fluorescence titration experiments revealed that complex 1 could act as multifunctional luminescent sensor to simultaneously detect UO22+, Cr2O72- and CrO42-, and NFT (nitrofurantoin). The limit of detection (LOD) values for complex 1 are 2.86 × 10-5, 4.09 × 10-5, 3.79 × 10-5 and 9.32 × 10-5 M for UO22+, Cr2O72-, CrO42- and NFT. The Ksv values are 6.18 × 103, 1.44 × 104, 1.27 × 104 and 1.51 × 104 M-1 for NFT, CrO42-, Cr2O72- and UO22+. Finally, the mechanism of its luminescence sensing is studied in detail. These results manifest that complex 1 is a multifunctional sensor for sensitive fluorescent UO22+, Cr2O72-, CrO42- and NFT detection.

5.
Front Chem ; 11: 1189308, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37179780

RESUMO

The speciation of epinephrine (Eph -) in the presence of alginate (Alg 2-) and two biological and environmental relevant metal cations (Cu2+, UO2 2+) was investigated at T = 298.15K, I = 0.15-1.00 mol dm-3 in NaCl(aq). The formation of binary and ternary complexes was evaluated and, since epinephrine can behave as a zwitterion, the Eph -/Alg 2- interaction was studied by means of DOSY NMR. The dependence of the equilibrium constants on ionic strength was studied using an extended Debye-Hückel type equation and the SIT approach. The effect of temperature was investigated by means of isoperibolic titration calorimetry: the entropic contribution was the driving force for the Cu2+/Eph - complexes formation. The sequestering ability of Eph - and Alg 2- on Cu2+, evaluated by the pL0.5 calculation, increased with pH and ionic strength. The determination of pM parameter showed that Eph - had a higher Cu2+ affinity with respect to Alg 2-. The formation of Eph -/Alg 2- species was also investigated by UV-Vis spectrophotometry and 1H NMR measurements. The ternary Cu2+/Eph -/Alg 2- and Cu2+/UO2 2+/Eph - interactions were also studied. The "extra-stability" calculated for the mixed ternary species confirmed that their formation was thermodynamically favorable.

6.
Adv Sci (Weinh) ; 10(13): e2300408, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36859764

RESUMO

Both proton exchange membrane fuel cells and uranium-based nuclear techniques represent two green and advanced energies. However, both of them still face some intractable scientific and industrial problems. For the former, established proton-conduction materials always suffer one or another defect such as low proton conductivity, high activation energy, bad durability, or just small-scale product; while for the later, there still lacks available adsorbent to selectively recover of UO2 2+ from concentrated nitric acid (>1 M) during the spent fuel reprocessing due to the deactivation of the adsorption site or the decomposition of adsorbent under such rigorous conditions. It is found that the above two issues can be well solved by the construction of sulfonic-pendent vinylene-linked covalent organic frameworks (COFs), since these COFs contain abundant sulfonic units for both intrinsic proton conduction and UO2 2+ capture through strong coordination fixation and vinylene linkage that enhances the stability up to 12 M nitric acid (one of the best materials surviving in 12 M HNO3 ).

7.
J Hazard Mater ; 445: 130442, 2023 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-36436454

RESUMO

It has been considered challenging to develop ideal adsorbents for efficient and lower adsorption time uranium extraction, especially 3D covalent organic frameworks with interpenetrating topologies and tunable porous structures. Here, a "soft" three-dimensional (3D) covalent organic framework (TAM-DHBD) with a fivefold interpenetrating structure is prepared as a novel porous platform for the efficient extraction of radioactive uranium. The resultant TAM-DHBD appears exceptional crystallinity, prominent porosity and excellent chemical stability. Based on the strong mutual coordination between phenolic-hydroxyl/imine-N on the main chain and uranium, TAM-DHBD can effectively avert the competition of other ions, showing high selectivity for uranium extraction. Impressively, the 3D ultra-hydrophilic transport channels and multi-directional uniform pore structure of TAM-DHBD lay the foundation for the ultra-high-speed diffusion of uranium (the adsorption equilibrium can be reached within 60 min under a high-concentration environment). Furthermore, the utilization of lightweight structure not only increases the adsorption site density, but renders the adsorption process flexible, achieving a breakthrough adsorption capacity of 1263.8 mg g-1. This work not only highlights new opportunities for designing microporous 3D COFs, but paves the way for the practical application of 3D COFs for uranium adsorption.

8.
Antibodies (Basel) ; 11(4)2022 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-36278614

RESUMO

Yeast surface display techniques have been increasingly employed as a tool for both the discovery and affinity maturation of antibodies. In this study, we describe the use of yeast surface display for the selection and affinity maturation of antibodies targeted to small molecules (haptens). In this approach, we coupled 4 to 15 sequential cycles of error-prone PCR to introduce heterogeneity into the sequence of an 12F6 scFv antibody that binds to chelated uranium; the resulting full-length constructs were combined to create a yeast-displayed scFv-library with high diversity. We also developed a stringent selection technique utilizing fluorescence-activated cell sorting; this was based on sequentially dropping the target antigen concentration, while concomitantly increasing the concentration of potential cross-reactive haptens in subsequent selection cycles. As a proof of the efficacy this approach, we confirmed that the antibodies identified via this approach retained binding to the target antigen (UO22+ complexed to a chelator), while binding with lesser affinity than the parental scFv to a structurally related haptens (the same chelator complexed to other metal ions). As will be described in this report, these scFv variants perform more efficiently in sensor-based assay than the parental 12F6 antibody. Combining the generation of scFv libraries via error-prone PCR with selection of yeast-displayed antibodies by fluorescence activated cell sorting will provide an efficient new method for the isolation of scFvs and other binding proteins with high affinity and specificity.

9.
Sensors (Basel) ; 22(18)2022 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-36146333

RESUMO

Developing a fluorescent probe for UO22+, which is resistant to interference from other ions such as Cu2+ and can be applied in acidic and high-water systems, has been a major challenge. In this study, a "turn-off" fluorescent probe for triamine-modified flavonoid derivatives, 2-triphenylamine-3-hydroxy-4H-chromen-4-one (abbreviated to HTPAF), was synthesized. In the solvent system of dimethyl sulfoxide:H2O (abbreviated to DMSO:H2O) (v/v = 5:95 pH = 4.5), the HTPAF solution was excited with 364 nm light and showed a strong fluorescence emission peak at 474 nm with a Stokes shift of 110 nm. After the addition of UO22+, the fluorescence at 474 nm was quenched. More importantly, there was no interference in the presence of metal ions (Pb2+, Cd2+, Cr3+, Fe3+, Co2+, Th4+, La3+, etc.), especially Cu2+ and Al3+. It is worth noting that the theoretical model for the binding of UO22+ to HTPAF was derived by more detailed density functional theory (DFT) calculations in this study, while the coordination mode was further verified using HRMS, FT-IR and 1HNMR, demonstrating a coordination ratio of 1:2. In addition, the corresponding photo-induced electron transfer (PET) fluorescence quenching mechanism was also proposed.


Assuntos
Corantes Fluorescentes , Água , Aminas/química , Cádmio , Dimetil Sulfóxido , Flavonoides , Corantes Fluorescentes/química , Íons , Chumbo , Solventes , Espectrometria de Fluorescência , Espectroscopia de Infravermelho com Transformada de Fourier
10.
Anal Chim Acta ; 1184: 338986, 2021 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-34625249

RESUMO

Herein, a dual-signal amplification electrochemical sensing has been proposed for the ultrasensitive detection of uranyl ions (UO22+) by integration of gold nanoparticles (AuNPs) and hybridization chain reaction (HCR)-assisted synthesis of silver nanoclusters (AgNCs). In this sensing platform, AuNPs are used as an ideal signal amplification carrier, aiming at increasing the loads of UO22+-specific DNAzyme on the gold electrode. In the presence of UO22+, UO22+-specific DNAzyme can be activated, leading to the cleavage of substrate strands (S-DNA). Then, HCR is triggered to produce long dsDNA through hybridization the probe with the ssDNA on the electrode surface. As a result, an amplified electrochemical response can be detected by inserting a large amount of AgNCs generated in situ using dsDNA as template. Featured with amplification efficiency, good specificity and high sensitivity, the strategy could quantitatively detect UO22+ down to 6.2 pM with a linear calibration range from 20 pM to 5000 pM. The proposed sensing platform has been also successfully demonstrated the practical application of detecting UO22+, indicating that the developed method has the potential applications and can open up a new avenue for highly sensitive detection of UO22+ in environmental monitoring.


Assuntos
Ouro , Nanopartículas Metálicas , Técnicas Eletroquímicas , Íons , Prata
11.
Int J Biol Macromol ; 183: 1640-1648, 2021 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-34044032

RESUMO

The present paper describes a green and cost-effective approach to investigate chitosan-sepiolite (Ch-Sep) composite as an adsorbent for removal of UO22+ ions in aqueous solution. The Ch-Sep composite was prepared as a beads using with two cross-linking agents: tripolyphosphate (TPP) and epichlorohydrin (ECH). Their adsorption properties for the removal of UO22+ ions in aqueous solution by batch experimental conditions were studied. The adsorptive removal processes of UO22+ ions from aqueous solution were evaluated by Langmuir, Freundlich and Dubinin-Radushkevich isotherm models, and was found to be perfectly fit to the Langmuir model (R2 = 0.971). The maximum adsorption capacity was 0.220 mol kg-1 at 25 °C from Langmuir isotherm model. Adsorption energy was 12.1 kJ mol-1 indicating that the adsorption process was chemical. The adsorption kinetics followed the pseudo second order and intra particle diffusion models. The thermodynamics parameters of UO22+ ions removal from aqueous solution was confirmed spontaneous, endothermic and possible at higher temperatures behavior of adsorption process. The adsorption mechanism of UO22+ ions onto Ch-Sep composite beads was investigated by FT-IR and SEM analysis. These findings revealed the effectiveness and potential of the newly synthesized Ch-Sep composite beads for the removal of UO22+ ions.


Assuntos
Quitosana/química , Silicatos de Magnésio/química , Urânio/análise , Poluentes Químicos da Água/análise , Adsorção , Reagentes de Ligações Cruzadas/química , Concentração de Íons de Hidrogênio , Íons , Cinética , Microscopia Eletrônica de Varredura , Espectroscopia de Infravermelho com Transformada de Fourier , Termodinâmica , Purificação da Água
12.
ACS Appl Mater Interfaces ; 13(11): 13883-13895, 2021 Mar 24.
Artigo em Inglês | MEDLINE | ID: mdl-33689268

RESUMO

The binary nanocomposites of metal/covalent-organic frameworks (NH2-MIL-125(Ti)@TpPa-1) were constructed by solvothermal method, which was developed as a multifunctional platform with adsorption and photocatalysis for radionuclides removal. The batch experiments and physicochemical property (FT-IR, XRD, SEM, TEM, XPS, etc.) corroborated: (i) core-shell NH2-MIL-125(Ti)@TpPa-1 had a more stable, multilayer pore structure and abundant active functional groups; (ii) NH2-MIL-125(Ti)@TpPa-1 had fast a removal rate, as well as a high adsorption capacity of 536.73 mg (UO22+)/g and 593.97 mg (Eu3+)/g; (iii) the pseudo-second-order and Langmuir model provided a more reasonable description, indicating the immobilization process was endothermic, spontaneous chemisorption; (iv) the adsorption mechanism was chelation and electrostatic attraction, ascribed to the nitrogen/oxygen-containing functional groups. These results illustrated that NH2-MIL-125(Ti)@TpPa-1 was a prospective adsorbent for the remediation polluted by radionuclides. In addition, the research provided the theoretical basis for further investigation on the UO22+(VI) photoreduction.

13.
J Hazard Mater ; 407: 124729, 2021 04 05.
Artigo em Inglês | MEDLINE | ID: mdl-33333387

RESUMO

In this research, an Al-based metal-organic framework (MOFs), CAU-1 was prepared through complexation between 2-aminoterephthalic acid and Al (III) by solvothermal approach, and simple operation and cost-effective synthetic route. The objective was to immobilize the typical positive/negative radionuclide ions (UO22+/TcO4-) in aqueous solution. The synthesized CAU-1 was characterized by XRD, FT-IR, TGA, FESEM, TEM-SAED, pHpzc, XPS and N2 physisorption analysis. The structure of CAU-1 possessed excellent thermostability, rich functional groups (‒NH2 and ‒OH groups), as well as large surface area (1636.3 m2/g) and the micropore volume (0.51 m3/g). Furthermore, batch experiments demonstrated that CAU-1 with superior adsorption capacity was 648.37 (UO22+) mg/g and 692.33 (ReO4-) mg/g calculating from Langmuir isotherm model, respectively. Thermodynamic investigation showed the adsorption process was endothermic and spontaneous. In addition, the adsorption mechanism of ReO4- ion onto CAU-1 could be electrostatic attraction and chelation effect, while for UO22+ ion, was mainly chelation effect induced by nitrogen-containing and oxygen-containing functional groups. Hence, the inexpensive and high-capacity CAU-1 could be considered as a practical material for sequestrations of radioactive pollutants from water environment.

14.
Mikrochim Acta ; 187(5): 311, 2020 05 04.
Artigo em Inglês | MEDLINE | ID: mdl-32367432

RESUMO

A superior electrochemical biosensor was designed for the determination of UO22+ in aqueous solution by integration of DNAzyme and DNA-modified gold nanoparticle (DNA-AuNP) network structure. Key features of this method include UO22+ inducing the cleavage of the DNAzyme and signal amplification of DNA-AuNP network structure. In this electrochemical method, the DNA-AuNP network structure can be effectively modified on the surface of gold electrode and then employed as an ideal signal amplification unit to generate amplified electrochemical response by inserting a large amount of electrochemically active indicator methylene blue (MB). In the presence of UO22+, the specific sites on DNA-AuNP network structure can be cleaved by UO22+, releasing the DNA-AuNP network structure with detectable reduction of electrochemical response intensity. The electrochemical response intensity is related to the concentration of UO22+. The logarithm of electrochemical response intensity and UO22+ concentration showed a wide linear range of 10~100 pM, and the detection limit reached 8.1 pM (S/N = 3). This method is successfully used for determination of UO22+ in water samples. Graphical abstract Fabricated DNAzyme network structure for enhanced electrical signal. Numerical experiments show that the current signal decreases as the concentration of UO22+ increases. It can be seen that the biosensors could be used to detect UO22+ in aqueous solution effectively.


Assuntos
Técnicas Biossensoriais/métodos , DNA Catalítico/química , Técnicas Eletroquímicas/métodos , Nanopartículas Metálicas/química , Compostos de Urânio/análise , Poluentes Químicos da Água/análise , Água Potável/análise , Ouro/química , Ácidos Nucleicos Imobilizados/química , Limite de Detecção , Azul de Metileno/química , Reprodutibilidade dos Testes , Rios/química , Compostos de Urânio/química , Poluentes Químicos da Água/química
15.
J Environ Radioact ; 205-206: 93-100, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31121425

RESUMO

The UO22+ biosorption properties of a lichen, Evernia prunastri, from aqueous solutions were investigated. The widely occurring lichen samples were collected from the forest in Bilecik-Turkey. The UO22+ biosorption onto lichen was characterized by FT-IR and SEM-EDX analysis techniques before and after biosorption. The effects of the solution pH, biosorbent dosage, UO22+ concentration, contact time, and temperature on UO22+ biosorption on lichen sample were studied by using the batch method. The isotherm experimental data were described using isotherm models of Langmuir, Freundlich and Dubinin Radushkevich. The maximum UO22+ biosorption capacity of the lichen sample was estimated by the Langmuir equation to be 0.270 mol kg-1. The adsorption energy from the Dubin Radushkevich model was found to be 8.24 kJ mol-1. Kinetic data determined that the biosorption was best described by the pseudo-second-order kinetic model. Thermodynamic findings showed that the biosorption process was endothermic, entropy increased and spontaneous. In conclusion, the lichen appears to be a promising biosorbent for the removal of UO22+ ions from aqueous solutions because of high biosorption capacity, easy usability, low cost, and high reusability performance.


Assuntos
Recuperação e Remediação Ambiental/métodos , Parmeliaceae/metabolismo , Compostos de Urânio/metabolismo , Poluentes Radioativos da Água/metabolismo , Adsorção , Biodegradação Ambiental , Biomassa , Cinética , Termodinâmica
16.
Nanomaterials (Basel) ; 9(5)2019 May 02.
Artigo em Inglês | MEDLINE | ID: mdl-31052588

RESUMO

Uranyl ion, the most soluble toxic uranium species, is recognized as an important index for monitoring nuclear wastewater quality. The United States Environmental Protection Agency (US EPA) and the World Health Organization (WHO) prescribed 30 ppb as the allowable concentration of uranyl ion in drinking water. This paper reports on a nanohybrid material that can detect uranyl ions spectroscopically and act as a uranyl ion absorbent in an aqueous system. Compound 1, possessing a salicyladazine core and four acetic acid groups, was synthesized and the spectroscopic properties of its UO22+ complex were studied. Compound 1 had a strong blue emission when irradiated with UV light in the absence of UO22+ that was quenched in the presence of UO22+. According to the Job's plot, Compound 1 formed a 1:2 complex with UO22+. When immobilized onto mesoporous silica, a small dose (0.3 wt %) of this hybrid material could remove 96% of UO22+ from 1 mL of a 100-ppb UO22+ aqueous solution.

17.
Chemosphere ; 223: 351-357, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-30784741

RESUMO

At the Department of Energy (DOE) managed Savannah River Site (SRS), uranium and other heavy metals continue to pose threats to the ecosystem health and processes. In the oxic soil of this site, uranium is present primarily as soluble salts of the uranyl ion (i.e., U(VI) or UO22+). Although UO22+ has a strong sorption to the soil, the mobile indigenous bacteria may facilitate its transport. On the contrary, precipitation of UO22+ with phosphate has been found to be an alternative remediation strategy. This research investigated the effects of mobile bacteria and phytate on UO22+ transport at SRS in column experiments. It was discovered that UO22+ can barely be mobilized by de-ionized water but can be significantly transported with the aid of mobile indigenous bacteria. UO22+ had the most facilitated transport observation when it reached equilibrium with the bacteria before the transport. When UO22+ and bacterial were introduced to the soil at the same time or UO22+ was pre-deposited in the soil, the facilitated transport was less pronounced. In the presence of phytate, bacterial-facilitated UO22+ transport was hindered. pH was found to play the key role for UO22+ immobilization in the presence of phytate. The immobilization of UO22+ with the addition of phytate increased with the increase of pH within the pH range of this study because of the impact of pH on the solubility of UO2(OH)2. Phytate promoted UO2--PO43- complex and/or [Ca(UO2)2(PO4)2] formation, leading to enhanced UO22+ immobilization in the SRS soil.


Assuntos
Bactérias/metabolismo , Ácido Fítico/farmacologia , Rios/química , Urânio/análise , Concentração de Íons de Hidrogênio , Imobilização , Fosfatos/química , Solo/química , Solubilidade , Compostos de Urânio/química
18.
Talanta ; 185: 258-263, 2018 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-29759198

RESUMO

Various DNA-modulated photosensitization schemes have been reported for various applications, but DNAzyme has not yet been included. Here, we found the DNAzyme with metal ion as cofactor could also be efficient in modulation of photosensitization process. The UO22+-specific DNAzyme can switch between double strand DNA (dsDNA) and single strand DNA (ssDNA) upon UO22+ cleavage, which can regulate the photosensitization process of SYBR Green I. Coupling with photosensitization-induced chromogenic reaction (TMB oxidation), a simple colorimetric sensor for UO22+ was developed accordingly. To increase the visual resolution of the proposed assay, a background color was supplied. Compared with the previous DNAzyme-based UO22+ sensors, the proposed assay featured label-free and simple. Besides, the tolerance for high salinity of this assay is appealing. The proposed assay offered a detection limit of 0.08 µg/L with UV-vis detection and 0.5 µg/L with the naked eye. With the proposed colorimetric assay, UO22+ levels in the range of 0.7-1.2 µg/L (2.9-5.0 nM) were identified in high salinity seawater samples, with spike-recoveries ranging from 93% to 104%.


Assuntos
Técnicas Biossensoriais , Colorimetria , DNA Catalítico/metabolismo , Água do Mar/química , Compostos de Urânio/análise , DNA Catalítico/química , Transtornos de Fotossensibilidade
19.
J Colloid Interface Sci ; 510: 280-291, 2018 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-28957744

RESUMO

Ag2O nanoparticles anchored on the Mg(OH)2 nanoplates (Ag2O@Mg(OH)2) were successfully prepared by a facile one-step method, which combined the Mg(OH)2 formation with Ag2O deposition. The synthesized products were characterized by a wide range of techniques including powder X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), selected area electron diffraction (SAED), and nitrogen physisorption analysis. It was found that Ag2O nanoparticles anchored on the Mg(OH)2 nanoplates show good dispersion and less aggregation relative to the single Ag2O nanoaggregates. In addition, iodide (I-) removal by the Ag2O@Mg(OH)2 nanocomposite was studied systematically. Batch experiments reveal that the nanocomposite exhibits extremely high I- removal rate (<10min), and I- removal capacity is barely affected by the concurrent anions, such as Cl-, SO42-, CO32- and NO3-. Furthermore, I- and UO22+ could be simultaneously removed by the nanocomposite with high efficiency. Due to the simple synthetic procedure, the excellent removal performances for iodine and uranium, and the easy separation from water, the Ag2O@Mg(OH)2 nanocomposite has real potential for application in radioactive wastewater treatment, especially during episodic environmental crisis.

20.
Spectrochim Acta A Mol Biomol Spectrosc ; 169: 208-15, 2016 Dec 05.
Artigo em Inglês | MEDLINE | ID: mdl-27380304

RESUMO

In this paper, two kinds of salophens (Sal) with different solubilities, Sal1 and Sal2, have been respectively synthesized, and they all can combine with uranyl to form stable complexes: [UO2(2+)-Sal1] and [UO2(2+)-Sal2]. Among them, [UO2(2+)-Sal1] was used as ligand to extract uranium in complex samples by dual cloud point extraction (dCPE), and [UO2(2+)-Sal2] was used as catalyst for the determination of uranium by photocatalytic resonance fluorescence (RF) method. The photocatalytic characteristic of [UO2(2+)-Sal2] on the oxidized pyronine Y (PRY) by potassium bromate which leads to the decrease of RF intensity of PRY were studied. The reduced value of RF intensity of reaction system (ΔF) is in proportional to the concentration of uranium (c), and a novel photo-catalytic RF method was developed for the determination of trace uranium (VI) after dCPE. The combination of photo-catalytic RF techniques and dCPE procedure endows the presented methods with enhanced sensitivity and selectivity. Under optimal conditions, the linear calibration curves range for 0.067 to 6.57ngmL(-1), the linear regression equation was ΔF=438.0 c (ngmL(-1))+175.6 with the correlation coefficient r=0.9981. The limit of detection was 0.066ngmL(-1). The proposed method was successfully applied for the separation and determination of uranium in real samples with the recoveries of 95.0-103.5%. The mechanisms of the indicator reaction and dCPE are discussed.

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