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1.
ACS Appl Mater Interfaces ; 13(37): 43937-43951, 2021 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-34499462

RESUMO

Nanotechnology has emerged as a promising solution to permanent elimination of cancer. However, nanoparticles themselves lack specificity to tumors. Due to enhanced migration to tumors, mesenchymal stem cells (MSCs) were suggested as cell-mediated delivery vehicles of nanoparticles. In this study, we have constructed a complex composed of photoluminescent quantum dots (QDs) and a photosensitizer chlorin e6 (Ce6) to obtain multifunctional nanoparticles, combining cancer diagnostic and therapeutic properties. QDs serve as energy donors-excited QDs transfer energy to the attached Ce6 via Förster resonance energy transfer, which in turn generates reactive oxygen species. Here, the physicochemical properties of the QD-Ce6 complex and singlet oxygen generation were measured, and the stability in protein-rich media was evaluated, showing that the complex remains the most stable in protein-free medium. In vitro studies on MSC and cancer cell response to the QD-Ce6 complex revealed the complex-loaded MSCs' potential to transport theranostic nanoparticles and induce cancer cell death. In vivo studies proved the therapeutic efficacy, as the survival of tumor-bearing mice was statistically significantly increased, while tumor progression and metastases were slowed down.


Assuntos
Antineoplásicos/uso terapêutico , Carcinoma Pulmonar de Lewis/diagnóstico por imagem , Carcinoma Pulmonar de Lewis/tratamento farmacológico , Células-Tronco Mesenquimais/metabolismo , Nanopartículas Multifuncionais/uso terapêutico , Animais , Antineoplásicos/química , Antineoplásicos/metabolismo , Antineoplásicos/efeitos da radiação , Compostos de Cádmio/química , Compostos de Cádmio/metabolismo , Compostos de Cádmio/efeitos da radiação , Compostos de Cádmio/uso terapêutico , Carcinoma Pulmonar de Lewis/metabolismo , Linhagem Celular Tumoral , Clorofilídeos/química , Clorofilídeos/metabolismo , Clorofilídeos/efeitos da radiação , Clorofilídeos/uso terapêutico , Feminino , Humanos , Luz , Camundongos Endogâmicos C57BL , Nanopartículas Multifuncionais/química , Nanopartículas Multifuncionais/metabolismo , Nanopartículas Multifuncionais/efeitos da radiação , Fotoquimioterapia/métodos , Fármacos Fotossensibilizantes/química , Fármacos Fotossensibilizantes/metabolismo , Fármacos Fotossensibilizantes/efeitos da radiação , Fármacos Fotossensibilizantes/uso terapêutico , Medicina de Precisão/métodos , Pontos Quânticos/química , Pontos Quânticos/metabolismo , Pontos Quânticos/efeitos da radiação , Pontos Quânticos/uso terapêutico , Compostos de Selênio/química , Compostos de Selênio/metabolismo , Compostos de Selênio/efeitos da radiação , Compostos de Selênio/uso terapêutico , Oxigênio Singlete/metabolismo , Sulfetos/química , Sulfetos/metabolismo , Sulfetos/efeitos da radiação , Sulfetos/uso terapêutico , Compostos de Zinco/química , Compostos de Zinco/metabolismo , Compostos de Zinco/efeitos da radiação , Compostos de Zinco/uso terapêutico
2.
J Am Chem Soc ; 143(36): 14635-14645, 2021 09 15.
Artigo em Inglês | MEDLINE | ID: mdl-34410692

RESUMO

Antibodies are recognition molecules that can bind to diverse targets ranging from pathogens to small analytes with high binding affinity and specificity, making them widely employed for sensing and therapy. However, antibodies have limitations of low stability, long production time, short shelf life, and high cost. Here, we report a facile approach for the design of luminescent artificial antibodies with nonbiological polymeric recognition phases for the sensitive detection, rapid identification, and effective inactivation of pathogenic bacteria. Transition-metal dichalcogenide (TMD) nanosheets with a neutral dextran phase at the interfaces selectively recognized S. aureus, whereas the nanosheets bearing a carboxymethylated dextran phase selectively recognized E. coli O157:H7 with high binding affinity. The bacterial binding sites recognized by the artificial antibodies were thoroughly identified by experiments and molecular dynamics simulations, revealing the significance of their multivalent interactions with the bacterial membrane components for selective recognition. The luminescent WS2 artificial antibodies could rapidly detect the bacteria at a single copy from human serum without any purification and amplification. Moreover, the MoSe2 artificial antibodies selectively killed the pathogenic bacteria in the wounds of infected mice under light irradiation, leading to effective wound healing. This work demonstrates the potential of TMD artificial antibodies as an alternative to antibodies for sensing and therapy.


Assuntos
Antibacterianos/uso terapêutico , Infecções por Escherichia coli/tratamento farmacológico , Substâncias Luminescentes/uso terapêutico , Nanoestruturas/uso terapêutico , Animais , Antibacterianos/química , Antibacterianos/efeitos da radiação , Dextranos/química , Escherichia coli O157/efeitos dos fármacos , Escherichia coli O157/isolamento & purificação , Luz , Substâncias Luminescentes/química , Substâncias Luminescentes/efeitos da radiação , Camundongos , Simulação de Dinâmica Molecular , Molibdênio/química , Molibdênio/efeitos da radiação , Molibdênio/uso terapêutico , Nanoestruturas/química , Nanoestruturas/efeitos da radiação , Terapia Fototérmica , Compostos de Selênio/química , Compostos de Selênio/efeitos da radiação , Compostos de Selênio/uso terapêutico , Pele/microbiologia , Análise Espectral Raman , Staphylococcus aureus/efeitos dos fármacos , Staphylococcus aureus/isolamento & purificação , Sulfetos/química , Sulfetos/efeitos da radiação , Sulfetos/uso terapêutico , Compostos de Tungstênio/química , Compostos de Tungstênio/efeitos da radiação , Compostos de Tungstênio/uso terapêutico , Cicatrização/efeitos dos fármacos
3.
J Radiat Res ; 62(5): 825-832, 2021 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-33998657

RESUMO

The accurate measurement of the 3D dose distribution of carbon-ion beams is essential for safe carbon-ion therapy. Although ionization chambers scanned in a water tank or air are conventionally used for this purpose, these measurement methods are time-consuming. We thus developed a rapid 3D dose-measurement tool that employs a silver-activated zinc sulfide (ZnS) scintillator with lower linear energy transfer (LET) dependence than gadolinium-based (Gd) scintillators; this tool enables the measurement of carbon-ion beams with small corrections. A ZnS scintillator sheet was placed vertical to the beam axis and installed in a shaded box. Scintillation images produced by incident carbon-ions were reflected with a mirror and captured with a charge-coupled device (CCD) camera. A 290 MeV/nucleon mono-energetic beam and spread-out Bragg peak (SOBP) carbon-ion passive beams were delivered at the Gunma University Heavy Ion Medical Center. A water tank was installed above the scintillator with the water level remotely adjusted to the measurement depth. Images were recorded at various water depths and stacked in the depth direction to create 3D scintillation images. Depth and lateral profiles were analyzed from the images. The ZnS-scintillator-measured depth profile agreed with the depth dose measured using an ionization chamber, outperforming the conventional Gd-based scintillator. Measurements were realized with smaller corrections for a carbon-ion beam with a higher LET than a proton. Lateral profiles at the entrance and the Bragg peak depths could be measured with this tool. The proposed method would make it possible to rapidly perform 3D dose-distribution measurements of carbon-ion beams with smaller quenching corrections.


Assuntos
Radioterapia com Íons Pesados , Imageamento Tridimensional/instrumentação , Radiometria/instrumentação , Sulfetos/efeitos da radiação , Compostos de Zinco/efeitos da radiação , Relação Dose-Resposta à Radiação , Desenho de Equipamento , Imageamento Tridimensional/métodos , Transferência Linear de Energia , Radiometria/métodos , Água
4.
Phys Chem Chem Phys ; 23(5): 3351-3360, 2021 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-33502403

RESUMO

The development of photocatalysts with high catalytic activity that are capable of full utilization of solar energy is a challenge in the field of photocatalysis. Accordingly, in the present study, an efficient Z-scheme cage-structured Co9S8/g-C3N4 (c-CSCN) photocatalyst was constructed for the degradation of tetracycline antibiotics under visible-light irradiation. The Z-scheme charge-transfer mechanism accelerates the separation of photogenerated charge carriers and effectively improves photocatalytic activity. Moreover, c-CSCN has a hollow structure, allowing light to be reflected multiple times inside the cavity, thereby effectively improving the utilisation efficiency of solar energy. As a result, the photocatalytic activity of c-CSCN is 1.5-, 2.5-, and 5.8-times higher than those of sheet-type Co9S8/g-C3N4 (s-CSCN), c-Co9S8, and g-C3N4, respectively, for the degradation of tetracycline. c-CSCN maintains favourable photocatalytic activity over five consecutive degradation cycles, demonstrating its excellent stability. In addition, c-CSCN performs efficient tetracycline removal in different water substrates. Moreover, c-CSCN exhibits excellent ability to remove tetracycline under direct natural sunlight. This work fully demonstrates that c-CSCN has high catalytic activity and the potential for practical application as a wastewater treatment material.


Assuntos
Antibacterianos/química , Cobalto/química , Grafite/química , Compostos de Nitrogênio/química , Sulfetos/química , Tetraciclina/química , Poluentes Químicos da Água/química , Catálise/efeitos da radiação , Cobalto/efeitos da radiação , Grafite/efeitos da radiação , Luz , Modelos Químicos , Compostos de Nitrogênio/efeitos da radiação , Sulfetos/efeitos da radiação
5.
Mikrochim Acta ; 187(8): 481, 2020 08 02.
Artigo em Inglês | MEDLINE | ID: mdl-32743681

RESUMO

A new fluorescence turn-on sensing platform has been developed applicable for sensitive profiling of multiple chemical and biological analytes, using azobenzene-quantum dot as a new stimuli-responsive optical nanoprobe. An azobenzene-carrying compound bis [4, 4'-(dithiophenyl azo)-1, 3-benzenediamine] (DTPABDA) is for the first time reported to be used for conjugation with CdSe/ZnS core/shell quantum dots (QDs) via the ligand exchange reaction. Due to the photo-induced electron-transfer (PET) effect, the electron-withdrawing azobenzene groups of DTPABDA can significantly cause the photoluminescence (PL) of QDs quenched. The QDs' PL can be subsequently reignited by the removal of azo moiety cleavable through three types of specific reactions: the dithionite reduction, hypochlorite oxidation, and azoreductase enzymatic catalysis, respectively. By monitoring of reaction-induced recovery of FL signals at 560 nm with an excitation of 450 nm, such azobenzene-QDs conjugates served as a new nanoprobe enabling the fluorescence turn-on sensing of dithionite, hypochlorite, and azoreductase with high sensitivity, broad linear range, and good selectivity. The successful detection of target analytes in real samples reveals the potential of our method in practical applications, such as biosensing, environmental and industrial monitoring. Graphical abstract A new stimuli-responsive fluorescence probe is reported for the sensitive detection of sodium dithionite, hypochlorite, and azoreductase. The probe consists of QDs with an azobenzene-carrying compound as a ligand. The fluorescence of QDs could be quenched by the azo group and subsequently recovered via the removal of azo group by these three compounds, resulting in the "turn-on" sensing of these compounds with high sensitivity, broad linear range, and good selectivity. The successful detection of azoreductase in serum samples reveals the practical use of this method.


Assuntos
Ditionita/análise , Corantes Fluorescentes/química , Ácido Hipocloroso/análise , Nitrorredutases/sangue , Pontos Quânticos/química , Compostos Azo/síntese química , Compostos Azo/química , Compostos de Cádmio/química , Compostos de Cádmio/efeitos da radiação , Corantes Fluorescentes/síntese química , Humanos , Luz , Limite de Detecção , Estudo de Prova de Conceito , Pontos Quânticos/efeitos da radiação , Compostos de Selênio/química , Compostos de Selênio/efeitos da radiação , Espectrometria de Fluorescência/métodos , Sulfetos/química , Sulfetos/efeitos da radiação , Compostos de Zinco/química , Compostos de Zinco/efeitos da radiação
6.
Mikrochim Acta ; 187(8): 450, 2020 07 16.
Artigo em Inglês | MEDLINE | ID: mdl-32676787

RESUMO

A photoelectrochemical (PEC) aptasensing platform is devised for sensitive detection of an organophosphorus pesticide based on dissolution of core-shell MnO2 nanoflower@CdS (MnO2 NF@CdS) by thiocholine (TCh). TCH is produced from the butyrylcholinesterase-acetylthiocholine system, accompanied by target-triggered rolling circle amplification (RCA). The core-shell MnO2 NF@CdS with excellent PEC performance was synthesized and employed as a photo-sensing platform. The target was detected on a functionalized magnetic probe with the corresponding aptamer. Upon malathion introduction, the aptamer was detached from the magnetic beads, while capture DNA (cDNA, with primer fragment) remained on the beads. The primer fragment in cDNA can trigger the RCA reaction to form a long single-stranded DNA (ssDNA). Furthermore, a large number of butyrylcholinesterase (BChE) were assembled on the long ssDNA strands through the hybridization with the S2-Au-BChE probe. Thereafter, TCh generated from hydrolysis of ATCh by BChE can reduce MnO2 NF (core) to Mn2+ and release the CdS nanoparticles (shell) from the platform electrode, significantly enhancing the PEC signal. Under optimal conditions, the proposed aptasensor exhibited high sensitivity for malathion with a low detection limit of 0.68 pg mL-1. Meanwhile, it also presents outstanding specificity, reproducibility, and stability. Importantly, the sensing platform provides a new concept for detection of pesticide. Graphical abstract Herein, this work devised a photoelectrochemical (PEC) aptasensing platform for sensitive detection of organophosphorus pesticide based on dissolution of core-shell MnO2 nanoflower@CdS (MnO2 NF@CdS) by the as-produced thiocholine (TCh) from the butyrylcholinesterase-acetylthiocholine system, accompanying with the target-triggered rolling circle amplification (RCA).


Assuntos
Técnicas Biossensoriais/métodos , Butirilcolinesterase/química , Malation/análise , Nanopartículas Metálicas/química , Praguicidas/análise , Animais , Aptâmeros de Nucleotídeos/química , Sequência de Bases , Compostos de Cádmio/química , Compostos de Cádmio/efeitos da radiação , Técnicas Eletroquímicas/métodos , Contaminação de Alimentos/análise , Sucos de Frutas e Vegetais/análise , Luz , Limite de Detecção , Fenômenos Magnéticos , Malation/química , Malus/química , Compostos de Manganês/química , Nanopartículas Metálicas/efeitos da radiação , Leite/química , Técnicas de Amplificação de Ácido Nucleico , Óxidos/química , Praguicidas/química , Processos Fotoquímicos , Sulfetos/química , Sulfetos/efeitos da radiação , Vinho/análise
7.
Anal Chem ; 92(16): 11476-11483, 2020 08 18.
Artigo em Inglês | MEDLINE | ID: mdl-32700529

RESUMO

Antibiotic resistance, encoded via particular genes, has become a major global health threat and substantial burden on healthcare. Hence, the facile, low-cost, and precise detection of antibiotic resistance genes (ARGs) is crucial in the realm of human health and safety, especially multiplex sensing assays. Here, a smart pH-regulated switchable photoelectrochemical (PEC) bioassay has been created for ultrasensitive detection of two typical subtypes of penicillin resistance genes bla-CTX-M-1 (target 1, labeled as TDNA1) and bla-TEM (target 2, labeled as TDNA2), whereby pH-responsive antimony tartrate (SbT) complex-grafted silica nanospheres are ingeniously adopted as signal DNA1 tags (labeled as SDNA1-SbT@SiO2NSs). The operations of the PEC bioassay depend on the switchable dissociation of the pH-responsive SDNA1-SbT@SiO2NSs complex under the external pH stimuli, thus initiating the pH-regulated release of ions pre-embedded in sandwich-type DNA nanoassemblies. At acidic conditions, the dissociation of SDNA1 tags (ON state) triggers the release of the embedded SbO+. Under alkaline conditions, the dissociation of SDNA1 tags is inhibited (OFF state). The detection of TDNA2 was achieved via DNA hybridization-triggered metal ion release. The unwinding of the introduced hairpin T-Hg2+-T fragment, hybridized with the second anchored signal DNA (SDNA2), ignites the release of Hg2+. The released SbO+ or Hg2+ ions would trigger the formation of Sb2S3/ZnS or HgS/ZnS heterostructure through ion-exchange with the photosensitive ZnS layer, giving rise to the amplified photocurrents and eventually realizing the ultrasensitive detection of penicillin resistance genes subtypes, bla-CTX-M-1 and bla-TEM. The as-fabricated pH-regulated PEC bioassay, smartly integrating the pH-responsive intelligent unit as SDNA tags, pH-regulated release of embedded ions, and the subsequent ion-exchange-based signal amplification strategy, exhibits high sensitivity, specificity, low-cost, and ease of use for multiplex detection of ARGs. It can be successfully used for measuring bla-CTX-M-1 and bla-TEM in real E. coli plasmids, demonstrating great promise for developing a new class of genetic point-of-care devices.


Assuntos
DNA Bacteriano/análise , Técnicas Eletroquímicas/métodos , Nanosferas , Fotoquímica/métodos , Antimônio/química , DNA Bacteriano/genética , Técnicas Eletroquímicas/instrumentação , Eletrodos , Escherichia coli/genética , Proteínas de Escherichia coli/genética , Genes Bacterianos/genética , Concentração de Íons de Hidrogênio , Nanopartículas de Magnetita/química , Resistência às Penicilinas/genética , Fotoquímica/instrumentação , Dióxido de Silício/química , Sulfetos/química , Sulfetos/efeitos da radiação , Tartaratos/química , Raios Ultravioleta , Compostos de Zinco/química , Compostos de Zinco/efeitos da radiação , beta-Lactamases/genética
8.
Analyst ; 145(13): 4436-4441, 2020 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-32469359

RESUMO

Anti-Stokes fluorescence induced by near-IR (NIR) radiation is particularly advantageous for the bioassay of complex samples, but most of the commonly used NIR-induced fluorescence nanomaterials such as up-conversion nanoparticles (UCNPs) do not exhibit satisfactory fluorescence intensity and work against achieving a highly sensitive bioassay. In this study, we a construct sensitive and specific bacteria biosensor based on the NIR-stimulated CaS: Eu, Sm, Mn and SrS: Ce, Sm, Mn nanoparticles. The fluorescent nanoparticles are conjugated with bacteria recognition fragments. In addition, the independent emission bands of these two types of fluorescent nanoparticles make it possible to detect and quantify Gram-positive strain and Gram-negative strain, simultaneously. Intense fluorescence and magnetic enrichment of magneto-fluorescence systems enable bacteria discrimination with the naked eye and improve sensitivity in trace bacteria detection (<20 CFU mL-1). The linear relationship between the fluorescence intensity and bacterial concentration is established with a detection range of 25-106 CFU mL-1. Furthermore, this NIR-excited assay strategy demonstrates better anti-interference capability than UV/visible-excited assay methods, showing high potential and practical value for medical diagnostics and bacteria monitoring.


Assuntos
Técnicas Bacteriológicas/métodos , Escherichia coli/isolamento & purificação , Corantes Fluorescentes/química , Nanopartículas Metálicas/química , Staphylococcus aureus/isolamento & purificação , Animais , Compostos de Cálcio/química , Compostos de Cálcio/efeitos da radiação , Escherichia coli/química , Fluorescência , Contaminação de Alimentos/análise , Raios Infravermelhos , Limite de Detecção , Fenômenos Magnéticos , Nanopartículas Metálicas/efeitos da radiação , Metais Pesados/química , Metais Pesados/efeitos da radiação , Microscopia de Fluorescência , Leite/microbiologia , Polimixina B/química , Espectrometria de Fluorescência , Staphylococcus aureus/química , Sulfetos/química , Sulfetos/efeitos da radiação , Teicoplanina/química
9.
Amino Acids ; 52(5): 841-845, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-32350627

RESUMO

The cysteine- perfluoroarene SNAr reaction allows for the sequence-specific attachment of dyes and affinity tags to peptides and proteins. However, while many methods exist for the desulfuration of native and functionalized cysteine residues, there are no reports of their application to perfluoroarylated cysteines. Herein we report both the hydrogenolysis of a perfluoroarylated cysteine to alanine and elimination to dehydroalanine, reactions that are both accelerated by microwave irradiation.


Assuntos
Cisteína/química , Éteres/química , Fluorocarbonos/química , Micro-Ondas , Fragmentos de Peptídeos/química , Sulfetos/química , Cisteína/efeitos da radiação , Éteres/efeitos da radiação , Fluorocarbonos/efeitos da radiação , Fragmentos de Peptídeos/efeitos da radiação , Sulfetos/efeitos da radiação
10.
Mikrochim Acta ; 187(6): 344, 2020 05 23.
Artigo em Inglês | MEDLINE | ID: mdl-32447460

RESUMO

Based on WS2 quantum dots (QDs) as fluorescent signals and MnO2 nanosheets as second-order scattering (SOS) signals, a combination of fluorescence and scattered light was used to construct a ratio sensing platform for glutathione (GSH) detection. When MnO2 nanosheets are added to WS2 QDs, the fluorescence of WS2 QDs is quenched by MnO2 nanosheets through IFE. Large-sized MnO2 nanosheets increase the SOS of the system and gradually approach the fluorescence. After adding GSH to WS2 QDs-MnO2, the MnO2 nanosheets were decomposed into Mn2+. The disappearance of the characteristic absorption peak of the MnO2 nanosheets suppressed the IFE to WS2 QDs, resulting in the fluorescence recovery of WS2 QDs. The reduction in size of MnO2 nanosheets after decomposition results in a decrease in the SOS of the system. Therefore, the ratio detection of GSH is obtained through the fluorescence and SOS dual signal response. Under optimal experimental conditions, the value of F406/S648 is linearly related to the GSH concentration in the range 0 to 60 µM, and the limit of detection (LOD) of GSH is 0.12 µM. In addition, the system is also used for the determination of GSH in real water samples and human serum, with good analytical results. Graphical abstract Schematic principle of fluorescence/scattered light system based on WS2 QDs-MnO2 for GSH ratiometric detection.


Assuntos
Corantes Fluorescentes/química , Glutationa/sangue , Compostos de Manganês/química , Óxidos/química , Pontos Quânticos/química , Espectrometria de Fluorescência/métodos , Água Potável/análise , Fluorescência , Corantes Fluorescentes/efeitos da radiação , Humanos , Limite de Detecção , Pontos Quânticos/efeitos da radiação , Sulfetos/química , Sulfetos/efeitos da radiação , Compostos de Tungstênio/química , Compostos de Tungstênio/efeitos da radiação
11.
J Hazard Mater ; 391: 121407, 2020 06 05.
Artigo em Inglês | MEDLINE | ID: mdl-32145925

RESUMO

In this work, a novel, economical and effective vessel-like biochar-based photocatalyst Bi2S3/BiOBr/BC was synthesized by a facile one-pot solvothermal method for the first time. A series of characterization analyses demonstrated the successful preparation of photocatalyst Bi2S3/BiOBr/BC. Furthermore, diclofenac (DCF) as the target contaminant was applied to elucidate the enhanced photocatalytic performance (93.65%, 40 min) under energy-saving visible LED light irradiation. Comparison experiments among different photocatalysts and photoelectrochemical tests results illustrated that excellent photocatalytic performance of Bi2S3/BiOBr/BC 10% might be attributed to the electrons transfer of biochar and higher charge separation efficiency of heterojunction structure. Besides, lower electrical energy per order value indicated photocatalyst/visible LED light system was more energy-saving. Proper photocatalyst dosage (0.6 g/L) and relatively acidic water environment (pH = 5.0) would be beneficial to DCF photodegrdation by Bi2S3/BiOBr/BC. Good reusability and stability of Bi2S3/BiOBr/BC were verified via five consecutive recycle experiments. Furthermore, the role of active species was determined through trapping experiments and O2- and h+ dominated the photodegradation reaction to mineralize DCF molecules. Eleven main intermediates and four possible photodegradation pathways were proposed by HRMS analysis. Accordingly, photocatalyst Bi2S3/BiOBr/BC would provide potential technical support for emerging pollutant removal in water matrix.


Assuntos
Anti-Inflamatórios não Esteroides/química , Bismuto/química , Carvão Vegetal/química , Diclofenaco/química , Sulfetos/química , Poluentes Químicos da Água/química , Catálise , Carvão Vegetal/efeitos da radiação , Técnicas Eletroquímicas , Luz , Processos Fotoquímicos , Sulfetos/efeitos da radiação
12.
Talanta ; 212: 120797, 2020 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-32113559

RESUMO

We report here sensitive photoelectrochemical immunosensing of Staphylococcus aureus (S. aureus) using ZnS-Ag2S/polydopamine (PDA) as a novel photoelectric material and Cu2O as the peroxidase mimic tag. ZnS-Ag2S heterojunctions were prepared on indium tin oxide (ITO) via electrodeposition of ZnS nanoparticles, followed by silver ion exchange. To prepare a PDA/ZnS-Ag2S/ITO, the ZnS-Ag2S/ITO electrode was coated with PDA by self-polymerization of dopamine. The photocurrent of the PDA/ZnS-Ag2S/ITO is 1.55 times that of the ZnS-Ag2S/ITO and 7.87 times that of the ZnS/ITO, indicating a high-performance photoelectric material. A sandwiched-type photoelectrochemical immunosensor was constructed by using PDA/ZnS-Ag2S/ITO as the photoelectrode and Cu2O nanocubes as the labels. Cu2O nanocubes can serve as peroxidase mimic to generate catalytic precipitates on the immunoelectrodes, and both the Cu2O nanocubes and the generated precipitates can decrease the photocurrents of the immunoelectrodes, so a photoelectrochemical immunosensor for detecting S. aureus was constructed, showing a linear range between 10 and 107 CFU mL-1 and a low detection limit of 2 CFU mL-1. Owing to the signal amplification of Cu2O labeling, the sensitivity of the Cu2O-labeled immunosensor is 4 times that of a label-free immunosensor for detecting S. aureus, and the detection limit (2 CFU mL-1) is lower than that of a label-free immunosensor (10 CFU mL-1). This work not only provides a new and efficient photoelectric material but also demonstrated an efficient signal-amplification strategy for photoelectrochemical biosensing.


Assuntos
Cobre/química , Imunoensaio/métodos , Indóis/química , Nanopartículas Metálicas/química , Polímeros/química , Staphylococcus aureus/isolamento & purificação , Anticorpos Imobilizados/imunologia , Técnicas Biossensoriais/métodos , Catálise , Técnicas Eletroquímicas/instrumentação , Técnicas Eletroquímicas/métodos , Eletrodos , Indóis/efeitos da radiação , Luz , Limite de Detecção , Nanopartículas Metálicas/efeitos da radiação , Polímeros/efeitos da radiação , Compostos de Prata/química , Compostos de Prata/efeitos da radiação , Staphylococcus aureus/imunologia , Sulfetos/química , Sulfetos/efeitos da radiação , Compostos de Estanho/química , Compostos de Zinco/química , Compostos de Zinco/efeitos da radiação
13.
J Hazard Mater ; 392: 122345, 2020 06 15.
Artigo em Inglês | MEDLINE | ID: mdl-32092644

RESUMO

Petal-like ZnS-SnS2 heterojunctions with Z-scheme band alignment were prepared by one-pot solvothermal strategy. The optimal (1:1) ZnS-SnS2 can degrade 93.46 % of tetracycline and remove 73.9 % COD of pharmaceutical wastewater under visible-light irradiation due to the efficient production of H, O2-, h+ and OH. The toxicity evaluation by ECOSAR prediction and the growth of E. coli indicates efficient toxicity reduction of tetracycline by photocatalysis and the non-toxicity of ZnS-SnS2. The attacked sites on tetracycline by reactive species were analyzed according to Fukui index, and two degradation pathways of tetracycline were inferred via the identification of intermediate products. Tetracycline degradation efficiency and the energy consumption in different water bodies were compared, and it was found that the electrical energy per order (EE/O) was the lowest in Ganjiang River. The valence band offset (ΔEVBO) and conduction band offset (ΔECBO) of ZnS-SnS2 were 1.02 eV and 0.22 eV, respectively. The probable photocatalytic mechanism of ZnS/SnS2 heterojunctions with Z-scheme band alignment based on ΔEVBO and ΔECBO was first presented.


Assuntos
Antibacterianos/química , Luz , Sulfetos/efeitos da radiação , Tetraciclina/química , Compostos de Estanho/efeitos da radiação , Poluentes Químicos da Água/química , Compostos de Zinco/efeitos da radiação , Antibacterianos/toxicidade , Catálise , Escherichia coli/efeitos dos fármacos , Escherichia coli/crescimento & desenvolvimento , Processos Fotoquímicos , Sulfetos/química , Tetraciclina/toxicidade , Compostos de Estanho/química , Eliminação de Resíduos Líquidos , Águas Residuárias , Purificação da Água , Compostos de Zinco/química
14.
J Hazard Mater ; 391: 122248, 2020 06 05.
Artigo em Inglês | MEDLINE | ID: mdl-32062348

RESUMO

Nowadays, increasing the risk for copper leaching into the drinking water in homes, hotels and schools has become unresolved issues all around the countries such as Canada, the United States, and Malaysia. The leaching of copper in tap water is due to a combination of acidic water, damaged pipes, and corroded plumbing fixtures. To remedy this global problem, a triple interconnected structure of CdS/Au/GQDs was designed as a photo-to-electron conversion medium for a real time and selective visible-light-prompt photoelectrochemical (PEC) sensor for Cu2+ ions in real water samples. The synergistic interaction of the CdS/Au/GQDs enabled the smooth transportation of charge carriers to the charge collector and provided a channel to inhibit the charge recombination reaction. Thus, a detection limit of 2.27 nM was obtained, which is 10,000 fold lower than that of WHO's Guidelines for Drinking-water Quality (∼30 µM). The photocurrent reduction was negligible after 30 days of storage under ambient conditions, suggesting the high stability of photoelectrode. Moreover, the real-time monitoring of Cu2+ ions in real samples was performed with satisfactory results, confirming the capability of the investigated photoelectrode as the most practical detector for trace amounts of Cu2+ ions.


Assuntos
Compostos de Cádmio/efeitos da radiação , Cobre/análise , Técnicas Eletroquímicas , Luz , Nanotubos/efeitos da radiação , Sulfetos/efeitos da radiação , Poluentes Químicos da Água/análise , Compostos de Cádmio/química , Cobre/química , Eletrodos , Ouro/química , Grafite/química , Nanotubos/química , Pontos Quânticos/química , Sulfetos/química , Poluentes Químicos da Água/química
15.
J Hazard Mater ; 384: 121308, 2020 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-31585292

RESUMO

There are increasing environmental concerns of serious pollution from emission of antibiotic wastewater. Herein, a series of direct Z-scheme WO2.72/ZnIn2S4 (WOZIS) hybrid photocatalysts composed of one-dimensional (1D) WO2.72 (WO) nanorods and two-dimensional (2D) ZnIn2S4 (ZIS) nanosheets have been designed and constructed for tetracycline hydrochloride (TCH) degradation without presence of solid-state electron mediators. The crystalline phase, chemical composition, morphology, optical properties and photocatalytic activity of the as-prepared samples were characterized by the XRD, XPS, SEM, HRTEM, BET, UV-vis DRS, and PL. Obviously, all the WOZIS hybrid photocatalysts exhibited significantly enhanced photocatalytic activity towards TCH degradation. Meanwhile, WOZIS-1 sample with WO/ZIS molar ratio of 1:1 showed the highest photocatalytic activity. The significantly enhanced photoactivity of WOZIS hybrid photocatalyst was due to Z-scheme charge separation mechanism based on the build of tight interfacial contacts between WO nanorods and ZIS nanosheets, thereby driving efficient charge separation. Moreover, the high photocatalytic stability of as-prepared WOZIS-1 hybrid sample was revealed through seven successive cycling reactions.


Assuntos
Antibacterianos/química , Nanotubos/química , Tetraciclina/química , Poluentes Químicos da Água/química , Catálise/efeitos da radiação , Índio/química , Índio/efeitos da radiação , Luz , Nanotubos/efeitos da radiação , Oxirredução , Fotólise , Sulfetos/química , Sulfetos/efeitos da radiação , Compostos de Tungstênio/química , Compostos de Tungstênio/efeitos da radiação , Águas Residuárias/química , Purificação da Água/métodos , Zinco/química , Zinco/efeitos da radiação
16.
J Hazard Mater ; 388: 121780, 2020 04 15.
Artigo em Inglês | MEDLINE | ID: mdl-31818661

RESUMO

Here a CdS embedded poly acrylic acid (PAA)/graphene oxide (GO) polymeric composite was prepared for the efficient degradation of chlortetracycline (CTC) driven by visible light irradiation. The structure-activity relationship of GO/PAA-CdS was confirmed through the photocatalytic evaluation of a series of samples prepared by varying GO concentration, molar ratio of Cd:S and the amount of crosslinking agent. Through the composition, morphology, photoelectrochemical characterizations and degradation kinetic studies, it could be confirmed that the enhanced photocatalytic activity is attributed to the controlled growth of CdS nanoparticles by polymer net structure and effective electron transfer along GO nanosheets. The photodegradation of CTC was confirmed to be mainly governed by O2- and OH radicals generated from GO/PAA-CdS. The degradation intermediates of CTC were confirmed by LC-MS, and possible degradation pathways were proposed based on the prediction of radical attacking sites according to Fukui function values obtained through Density Functional Theory (DFT). Moreover, it was found that the catalytic activity of the photocatalyst was maintained after several cycles confirming the enhanced anti-photocorrosion of GO/PAA-CdS. This research provided an efficient approach by a novel photocatalyst for the removal of CTC from wastewater.


Assuntos
Resinas Acrílicas , Antibacterianos/química , Compostos de Cádmio , Clortetraciclina/química , Grafite , Nanopartículas , Sulfetos , Resinas Acrílicas/química , Resinas Acrílicas/efeitos da radiação , Compostos de Cádmio/química , Compostos de Cádmio/efeitos da radiação , Precipitação Química , Grafite/química , Grafite/efeitos da radiação , Luz , Nanopartículas/química , Nanopartículas/efeitos da radiação , Fotólise , Sulfetos/química , Sulfetos/efeitos da radiação , Purificação da Água
17.
J Hazard Mater ; 384: 121438, 2020 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-31629600

RESUMO

In this study, a self-biased bio-photoelectrochemical system (SB-BPES) was constructed using a bioanode and the g-C3N4/CdS heterojunction photocathode for nitrofurazone (NFZ) degradation under solar irradiation. The physio-chemical properties and optical performance of photocatalysts were characterized, and photo-electrochemical properties of various photocathodes were analyzed. Results showed that g-C3N4/CdS exhibited the broadest visible light absorption range (to 594 nm) and the most efficient e--h+ separation; and its corresponding photocathode showed the highest photocurrent (9.8 µA), and the lowest charge transfer resistance (5.43 ☓ 103 Ω). In the solar-illuminated SB-BPES with g-C3N4/CdS photocathode, about 80% of NFZ removal rate was achieved within 10 h. More importantly, TOC removal of 62.6% was achieved in 24 h, which was 1.8 times of that from the open circuit SB-BPES, and 4.3 folds of that from microbial degradation; also, about 1.5 times of those from SB-BPES with g-C3N4 and CdS photocathodes. Besides, reproducible current generations (∼1.0 mA) were produced. These verified that it was a self-sustained system for spontaneously pollutants degradation and electricity generation. Moreover, possible degradation mechanism and pathways were proposed according to the identified intermediates. This study provides inspiration for synchronic improving refractory organics degradation and net energy recovery.


Assuntos
Anti-Infecciosos/química , Anti-Infecciosos/metabolismo , Compostos de Cádmio/química , Nitrilas/química , Nitrofurazona/química , Nitrofurazona/metabolismo , Sulfetos/química , Bactérias/metabolismo , Biodegradação Ambiental , Compostos de Cádmio/efeitos da radiação , Catálise , Técnicas Eletroquímicas , Nitrilas/efeitos da radiação , Fotólise , Sulfetos/efeitos da radiação , Luz Solar
18.
Mikrochim Acta ; 186(11): 692, 2019 10 12.
Artigo em Inglês | MEDLINE | ID: mdl-31605242

RESUMO

A photocathode is described for the determination of microRNA-21 by using CuInS2 as an active photocathode material. Exonuclease III assisted target recycling amplification was employed to enhance the detection sensitivity. The TATA-binding protein (TBP) was applied to enhance steric hindrance which decreases the photoelectrochemical intensity. This strategy is designed by combining the anti-interference photocathode material, enzyme assisted target recycling amplification and TBP induced signal off, showing remarkable amplification efficiency. Under the optimized conditions, the detection limit for microRNA-21 is as low as 0.47 fM, and a linear range was got from 1.0 × 10-15 M to 1.0 × 10-6 M. Graphical abstract Schematic representation of sensitive photoelectrochemical detection of microRNA-21.CuInS2 is used as an active photocathode material. Combined Exonuclease III assisted target recycling amplification and TATA-binding protein decreased of photoelectrochemical intensity, the detection limit was 0.47 fM with good selectivity. (miR-21: microRNA-21; CS: chitosan).


Assuntos
DNA/química , Técnicas Eletroquímicas/métodos , Exodesoxirribonucleases/química , MicroRNAs/sangue , Fotoquímica/métodos , Sulfetos/química , Aptâmeros de Nucleotídeos/química , Aptâmeros de Nucleotídeos/genética , Sequência de Bases , Biomarcadores Tumorais/sangue , Biomarcadores Tumorais/química , Biomarcadores Tumorais/genética , Cobre/química , Cobre/efeitos da radiação , DNA/genética , Técnicas Eletroquímicas/instrumentação , Eletrodos , Humanos , Índio/química , Índio/efeitos da radiação , Sequências Repetidas Invertidas , Luz , Limite de Detecção , MicroRNAs/química , MicroRNAs/genética , Hibridização de Ácido Nucleico , Sulfetos/efeitos da radiação , Compostos de Estanho/química
19.
Carbohydr Polym ; 222: 115039, 2019 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-31320053

RESUMO

The purpose of this study was to design an injectable hydrogel with temperature-sensitive property for safe and high efficient in vivo colon cancer hyperthermia and chemotherapy. Chitosan (CS) solution was injected into the tumor at room temperature and automatically gelled after warming to body temperature in the present of ß-glycerophosphate (ß-GP). Combined localized tumor photothermal and chemotherapy were achieved by dissolving photothermal material MoS2/Bi2S3-PEG (MBP) nanosheets and drug molecule doxorubicin (DOX) into the hydrogel, and the gel system could encapsulate DOX and MBP nanosheets and prevent them from entering the blood circulation and damaging normal tissues and cells. More importantly, the CS/MBP/DOX (CMD) hydrogel exhibited a photothermal efficiency of 22.18% and 31.42% in the first and second near infrared light (NIR I and NIR II) biowindows respectively at a low MBP concentration (0.5 mg/mL). Besides, the release of the DOX from CMD hydrogel was controllable since the gel temperature could be governed by NIR laser irradiation. Moreover, the chitosan-based hydrogel had antibacterial effects. The designed composite hydrogel is anticipated to act as a platform for the high efficient treatment of tumors owing to the different penetration depths of NIR I and NIR II.


Assuntos
Antineoplásicos/uso terapêutico , Quitosana/química , Neoplasias do Colo/tratamento farmacológico , Doxorrubicina/uso terapêutico , Portadores de Fármacos/química , Hidrogéis/química , Animais , Antibacterianos/administração & dosagem , Antibacterianos/química , Antibacterianos/farmacologia , Antineoplásicos/administração & dosagem , Bismuto/administração & dosagem , Linhagem Celular , Quitosana/administração & dosagem , Quitosana/farmacologia , Dissulfetos/administração & dosagem , Dissulfetos/efeitos da radiação , Doxorrubicina/administração & dosagem , Portadores de Fármacos/administração & dosagem , Portadores de Fármacos/farmacologia , Liberação Controlada de Fármacos , Escherichia coli/efeitos dos fármacos , Hidrogéis/administração & dosagem , Hidrogéis/farmacologia , Hipertermia Induzida/métodos , Raios Infravermelhos , Injeções , Camundongos Endogâmicos BALB C , Molibdênio/administração & dosagem , Molibdênio/efeitos da radiação , Polietilenoglicóis/administração & dosagem , Polietilenoglicóis/química , Sulfetos/administração & dosagem , Sulfetos/efeitos da radiação , Temperatura , Ensaios Antitumorais Modelo de Xenoenxerto
20.
Analyst ; 144(15): 4661-4666, 2019 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-31259991

RESUMO

A split-type photoelectrochemical immunosensor was designed for the ultrasensitive monitoring of prostate-specific antigen (PSA) based on a Cu2+-mediated catalytic reaction for inhibiting the in situ generation of CdS quantum dots (QDs) coupled with the enhancement of the CdS/MoS2 heterojunction; it was constructed by the stepwise modification of MoS2 QDs and CdS QDs onto an ITO electrode surface. In the presence of PSA, CuO NP-labeled anti-PSA antibodies were immobilized onto an anti-PSA antibody-modified 96-well plate via a sandwich immunoreaction and dissolution by hydrochloric acid to obtain a large number of Cu2+ ions. As the Cu2+-triggered catalytic oxidization of glutathione occurred, the in situ growth of CdS QDs as a signal indicator was significantly suppressed, resulting in reduction in the photocurrent response. Under optimal conditions, the biosensor exhibited desirable linearity in the range from 0.5 pg mL-1 to 10 ng mL-1, low detection limit of 0.29 pg mL-1, satisfactory selectivity, and good stability. It was applied to PSA detection in human serum, suggesting a great potential for early diagnostics of some cancers.


Assuntos
Cobre/química , Antígeno Prostático Específico/sangue , Pontos Quânticos/química , Anticorpos Imobilizados/imunologia , Técnicas Biossensoriais/métodos , Compostos de Cádmio/química , Compostos de Cádmio/efeitos da radiação , Dissulfetos/química , Técnicas Eletroquímicas/instrumentação , Técnicas Eletroquímicas/métodos , Eletrodos , Glutationa/química , Humanos , Imunoensaio/métodos , Luz , Limite de Detecção , Masculino , Molibdênio/química , Oxirredução , Processos Fotoquímicos , Antígeno Prostático Específico/imunologia , Pontos Quânticos/efeitos da radiação , Sulfetos/química , Sulfetos/efeitos da radiação , Compostos de Estanho/química
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