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1.
Nat Commun ; 15(1): 3459, 2024 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-38658566

RESUMO

Establishing dependable, cost-effective electrical connections is vital for enhancing device performance and shrinking electronic circuits. MXenes, combining excellent electrical conductivity, high breakdown voltage, solution processability, and two-dimensional morphology, are promising candidates for contacts in microelectronics. However, their hydrophilic surfaces, which enable spontaneous environmental degradation and poor dispersion stability in organic solvents, have restricted certain electronic applications. Herein, electrohydrodynamic printing technique is used to fabricate fully solution-processed thin-film transistors with alkylated 3,4-dihydroxy-L-phenylalanine functionalized Ti3C2Tx (AD-MXene) as source, drain, and gate electrodes. The AD-MXene has excellent dispersion stability in ethanol, which is required for electrohydrodynamic printing, and maintains high electrical conductivity. It outperformed conventional vacuum-deposited Au and Al electrodes, providing thin-film transistors with good environmental stability due to its hydrophobicity. Further, thin-film transistors are integrated into logic gates and one-transistor-one-memory cells. This work, unveiling the ligand-functionalized MXenes' potential in printed electrical contacts, promotes environmentally robust MXene-based electronics (MXetronics).

2.
Nanomicro Lett ; 15(1): 123, 2023 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-37160615

RESUMO

With an excellent power conversion efficiency of 25.7%, closer to the Shockley-Queisser limit, perovskite solar cells (PSCs) have become a strong candidate for a next-generation energy harvester. However, the lack of stability and reliability in PSCs remained challenging for commercialization. Strategies, such as interfacial and structural engineering, have a more critical influence on enhanced performance. MXenes, two-dimensional materials, have emerged as promising materials in solar cell applications due to their metallic electrical conductivity, high carrier mobility, excellent optical transparency, wide tunable work function, and superior mechanical properties. Owing to different choices of transition elements and surface-terminating functional groups, MXenes possess the feature of tuning the work function, which is an essential metric for band energy alignment between the absorber layer and the charge transport layers for charge carrier extraction and collection in PSCs. Furthermore, adopting MXenes to their respective components helps reduce the interfacial recombination resistance and provides smooth charge transfer paths, leading to enhanced conductivity and operational stability of PSCs. This review paper aims to provide an overview of the applications of MXenes as components, classified according to their roles as additives (into the perovskite absorber layer, charge transport layers, and electrodes) and themselves alone or as interfacial layers, and their significant importance in PSCs in terms of device performance and stability. Lastly, we discuss the present research status and future directions toward its use in PSCs.

3.
Nanomaterials (Basel) ; 13(5)2023 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-36903666

RESUMO

Pristine MXene films express outstanding excellent electromagnetic interference (EMI) shielding properties. Nevertheless, the poor mechanical properties (weak and brittle nature) and easy oxidation of MXene films hinder their practical applications. This study demonstrates a facile strategy for simultaneously improving the mechanical flexibility and the EMI shielding of MXene films. In this study, dicatechol-6 (DC), a mussel-inspired molecule, was successfully synthesized in which DC as mortars was crosslinked with MXene nanosheets (MX) as bricks to create the brick-mortar structure of the MX@DC film. The resulting MX@DC-2 film has a toughness of 40.02 kJ·m-3 and Young's modulus of 6.2 GPa, which are improvements of 513% and 849%, respectively, compared to those of the bare MXene films. The coating of electrically insulating DC significantly reduced the in-plane electrical conductivity from 6491 S·cm-1 for the bare MXene film to 2820 S·cm-1 for the MX@DC-5 film. However, the EMI shielding effectiveness (SE) of the MX@DC-5 film reached 66.2 dB, which is noticeably greater than that of the bare MX film (61.5 dB). The enhancement in EMI SE resulted from the highly ordered alignment of the MXene nanosheets. The synergistic concurrent enhancement in the strength and EMI SE of the DC-coated MXene film can facilitate the utilization of the MXene film in reliable, practical applications.

4.
ACS Nano ; 2022 Nov 14.
Artigo em Inglês | MEDLINE | ID: mdl-36374133

RESUMO

Ligands can control the surface chemistry, physicochemical properties, processing, and applications of nanomaterials. MXenes are the fastest growing family of two-dimensional (2D) nanomaterials, showing promise for energy, electronic, and environmental applications. However, complex oxidation states, surface terminal groups, and interaction with the environment have hindered the development of organic ligands suitable for MXenes. Here, we demonstrate a simple, fast, scalable, and universally applicable ligand chemistry for MXenes using alkylated 3,4-dihydroxy-l-phenylalanine (ADOPA). Due to the strong hydrogen-bonding and π-electron interactions between the catechol head and surface terminal groups of MXenes and the presence of a hydrophobic fluorinated alkyl tail compatible with organic solvents, the ADOPA ligands functionalize MXene surfaces under mild reaction conditions without sacrificing their properties. Stable colloidal solutions and highly concentrated liquid crystals of various MXenes, including Ti2CTx, Nb2CTx, V2CTx, Mo2CTx, Ti3C2Tx, Ti3CNTx, Mo2TiC2Tx, Mo2Ti2C3Tx, and Ti4N3Tx, have been produced in various organic solvents. Such products offer excellent electrical conductivity, improved oxidation stability, and excellent processability, enabling applications in flexible electrodes and electromagnetic interference shielding.

5.
ACS Nano ; 16(9): 13370-13429, 2022 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-36094932

RESUMO

Photocatalytic water splitting, CO2 reduction, and pollutant degradation have emerged as promising strategies to remedy the existing environmental and energy crises. However, grafting of expensive and less abundant noble-metal cocatalysts on photocatalyst materials is a mandatory practice to achieve enhanced photocatalytic performance owing to the ability of the cocatalysts to extract electrons efficiently from the photocatalyst and enable rapid/enhanced catalytic reaction. Hence, developing highly efficient, inexpensive, and noble-metal-free cocatalysts composed of earth-abundant elements is considered as a noteworthy step toward considering photocatalysis as a more economical strategy. Recently, MXenes (two-dimensional (2D) transition-metal carbides, nitrides, and carbonitrides) have shown huge potential as alternatives for noble-metal cocatalysts. MXenes have several excellent properties, including atomically thin 2D morphology, metallic electrical conductivity, hydrophilic surface, and high specific surface area. In addition, they exhibit Gibbs free energy of intermediate H atom adsorption as close to zero and less than that of a commercial Pt-based cocatalyst, a Fermi level position above the H2 generation potential, and an excellent ability to capture and activate CO2 molecules. Therefore, there is a growing interest in MXene-based photocatalyst materials for various photocatalytic events. In this review, we focus on the recent advances in the synthesis of MXenes with 2D and 0D morphologies, the stability of MXenes, and MXene-based photocatalysts for H2 evolution, CO2 reduction, and pollutant degradation. The existing challenges and the possible future directions to enhance the photocatalytic performance of MXene-based photocatalysts are also discussed.

6.
Front Chem ; 9: 734108, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34660530

RESUMO

Solar energy-driven carbon dioxide (CO2) reduction to valuable solar fuels/chemicals (e.g., methane, ethanol, and carbon monoxide) using particulate photocatalysts is regarded as one of the promising and effective approaches to deal with energy scarcity and global warming. The growth of nanotechnology plays an eminent role in improving CO2 reduction (CO2R) efficiencies by means of offering opportunities to tailor the morphology of photocatalysts at a nanoscale regime to achieve enhanced surface reactivity, solar light absorption, and charge separation, which are decisive factors for high CO2R efficiency. Notably, quantum dots (QDs), tiny pieces of semiconductors with sizes below 20 nm, offering a myriad of advantages including maximum surface atoms, very short charge migration lengths, size-dependent energy band positions, multiple exciton generation effect, and unique optical properties, have recently become a rising star in the CO2R application. In this review, we briefly summarized the progress so far achieved in QD-assisted CO2 photoreduction, highlighting the advantages of QDs prepared with diverse chemical compositions such as metal oxides, metal chalcogenides, carbon, metal halide perovskites, and MXenes.

7.
ACS Appl Mater Interfaces ; 13(29): 34648-34657, 2021 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-34279075

RESUMO

Limited light absorption beyond the UV region and rapid photocarrier recombination are critical impediments for the improved photocatalytic performance of carbon quantum dots (CQDs) under visible-light irradiation. Herein, we demonstrate single-step microwave-assisted syntheses of O-CQDs (typical CQDs terminated by carboxylic and hydroxyl functional groups) from a sucrose precursor and Cl-doped CQDs (Cl-CQDs) from a sucralose precursor in short reaction times and without using obligatory strong acids for Cl doping. The doping of Cl into the CQDs is observed to widen the absorption range and facilitate an enhanced separation of photoexcited charge carriers, which is confirmed by the results of optical absorption, photothermal response, and pump-probe ultrafast transient absorption spectroscopy measurements of the O-CQDs and Cl-CQDs. The photoexcited charge carriers with their longer lifetimes in Cl-CQDs enabled the quick degradation of methylene blue dye, rapid conversion of Ag+ ions to metallic Ag nanoparticles on the CQD surfaces, and reduction of GO to a well-dispersed rGO through the photoelectron transfer reactions under visible-light irradiation. The facile Cl doping strategy, hybridization of Ag nanoparticles or rGO to CQDs, and the elevated charge separation mechanism would open up new avenues in designing CQD-based materials for futuristic applications.

8.
Anal Chem ; 93(24): 8638-8646, 2021 06 22.
Artigo em Inglês | MEDLINE | ID: mdl-34110775

RESUMO

In situ wireless monitoring for cell proliferation and detachment kinetics was conducted using pH-responsive zwitterionic polymer dots (Z-PDs), based on changes in electrochemical signals derived from Z-PD-coated substrates via the interaction of charges transferred between Z-PDs and cells. Z-PD-coated substrates were found to be a potent means to monitor and manipulate cell adhesion and detachment because of their high sensitivity over a wide range of pH conditions, and modification of the coated substrates was confirmed using a wireless system. At neutral pH, Z-PD-coated wireless sensors exhibited π-π stacking involving aromatic rings with hydrophobic interactions, thereby promoting cell proliferation; consequently, an increase in the measured resistance was observed. In contrast, Z-PD-coated substrates triggered by acidic and basic conditions promoted cell detachment, which induced an increase in the resistance compared with Z-PD substrates at pH 6.8, as a result of charges transferred to support Z-PD internalization through cell membranes after detachment. Therefore, as a wireless biosensor with excellent pH responsiveness that facilitates cell proliferation and detachment and whose electrochemical signals could be additionally acquired via a smartphone, Z-PD biosensors demonstrated a more favorable approach for monitoring cell-surface interactions than conventional optically based methods.


Assuntos
Polímeros , Proliferação de Células , Condutividade Elétrica , Concentração de Íons de Hidrogênio , Interações Hidrofóbicas e Hidrofílicas
9.
ACS Appl Mater Interfaces ; 12(46): 51766-51775, 2020 Nov 18.
Artigo em Inglês | MEDLINE | ID: mdl-33146512

RESUMO

The reversible volume memories of the inner structures of soft materials with controllable hydrophilic-hydrophobic balance have been widely recognized, for example, hydrogels used in pressure sensors. Mechanical stimuli, such as pressure, vibration, and tensile, may influence the deformation of the hydrogel while simultaneously changing the electronic signal. Here, we designed a hydrophobic carbon dot nanoparticle (f-CD) mixed with polyvinyl alcohol and catechol-conjugated chitosan to obtain a hydrogel suitable for pressure and vibration sensor applications. The hydrophobicity of loaded f-CD plays an important role in mechanical performance and electronic signal acquisition. It also affects the different rheological reversibility and shape recovery as an impact on the volume transition. These characteristics are influenced by the compactness, dimensional structure, and density of the fabricated hydrogel. As a result, hydrogels with high hydrophobicity have a stiff structure (shear modulus 8123.1 N·m-2) compared to that of the hydrophilic hydrogel (ranging between 6065.7 and 7739.2 N·m-2). Moreover, the mechanically dependent volume transition hydrogel affects the electronic resistivity (up to 17.3 ± 1.3%) and capacitance change (up to 145%) when compressed with different forces. The hydrogel with a controlled hydrophobic-hydrophilic inner structure shows a unique sensitivity and great potential for various applications in wearable electronic skins, real-time clinical health-care monitoring, and human-computer interactions.


Assuntos
Carbono/química , Hidrogéis/química , Nanopartículas/química , Dispositivos Eletrônicos Vestíveis , Catecóis/química , Quitosana/química , Capacitância Elétrica , Humanos , Interações Hidrofóbicas e Hidrofílicas , Movimento/fisiologia , Reologia , Tecnologia sem Fio
10.
ACS Appl Mater Interfaces ; 12(30): 34105-34114, 2020 Jul 29.
Artigo em Inglês | MEDLINE | ID: mdl-32613826

RESUMO

We propose an integrated, self-powered, flexible electronic skin device containing an alginate-derived polymer dot (A-PD)-incorporated mineralized hydrogel-based energy storage unit and a chitosan-derived n-type carbon dot (N-CD)-based solar cell for an energy-harvesting unit. This study demonstrates a unique architecture of mineralized hydrogel comprising A-PD-incorporated poly(acrylic acid) (PAA)/CaCO3/laponite containing soft and sensitive layers, deposited with a polyaniline electrode to serve as an energy storage unit. The self-assembly was achieved through the ionic cross-linking between A-PD and PAA driven by the mineralization process, resulting in excellent dimensional stability and improved mechanical properties of the hydrogel. The sp2 carbon-rich A-PD enhances the electrochemical performance and the overall photon-to-electrical conversion and storage efficiency for self-powered devices by the formation of the bridge of electrons between the ionized polymer and metal ion. The capacitive sensor developed in this study exhibits high sensitivity in detecting small pressure changes, such as the falling of small water droplets. The self-powered sensing device can detect and monitor various human motions continuously by harvesting light energy from outdoor sunlight. Furthermore, the energy-autonomous device exhibits unique responses for handwriting characters stably and repeatedly. The proposed system may be applicable to human-machine interfaces, biomonitoring systems, secure communication, and wearable devices.


Assuntos
Resinas Acrílicas/química , Hidrogéis/química , Pontos Quânticos/química , Dispositivos Eletrônicos Vestíveis , Alginatos/química , Carbonato de Cálcio/química , Carbono/química , Quitosana/química , Eletrodos , Silicatos/química , Energia Solar
11.
ACS Appl Mater Interfaces ; 12(11): 13428-13436, 2020 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-32096621

RESUMO

Herein, we demonstrate the ultraviolet (UV) light activated high-performance room-temperature NO gas sensor based on nitrogen-doped graphene quantum dots (NGQDs)-decorated TiO2 hybrid structure. TiO2 employed in the form of {001} facets exposed rectangular nanoplate morphology, which is highly reactive for the adsorption of active oxygen species. NGQD layers are grown on TiO2 nanoplates by graphitization of precursors via hydrothermal treatment. The decoration of NGQDs on the TiO2 surface dramatically enhanced the efficiency of gas and carriers exchange, charge carrier separation and transportation, and oxygen vacancies, which eventually improved the sensing performance. At room temperature, the TiO2@NGQDs hybrid structure exhibited a response of 12.0% to 100 ppm NO, which is 4.8 times higher compared to that of pristine TiO2 nanoplates. The response of TiO2@NGQDs hybrid structure is further upgraded by employing the ultraviolet light illumination and manipulating the operating temperature. Under the UV (λ = 365 nm) illumination at room temperature, the hybrid structure response escalated to ∼31.1% for 100 ppm NO. On the other hand, the tailoring of working temperature yielded a response of ∼223% at an optimum operating temperature of 250 °C. The NO gas-sensing mechanism of TiO2@NGQDs nanoplate's hybrid structure sensors under UV illumination and different working temperatures is discussed.

12.
RSC Adv ; 10(16): 9245-9257, 2020 Mar 02.
Artigo em Inglês | MEDLINE | ID: mdl-35497234

RESUMO

Novel and effective reduced graphene oxide-nickel (Ni) doped manganese oxide (RGO/Ni-MnO2) adsorbents were fabricated via a hydrothermal approach. The reduction of graphite to graphene oxide (GO), formation of α-MnO2, and decoration of Ni-MnO2 onto the surface of reduced graphene oxide (RGO) were independently carried out by a hydrothermal technique. The physical and morphological properties of the as-synthesized adsorbents were analyzed. Batch adsorption experiments were performed to identify the lithium uptake capacities of adsorbents. The optimized parameters for Li+ adsorption investigated were pH = 12, dose loading = 0.1 g, Li+ initial concentration = 50 mg L-1, in 10 h at 25 °C. It is noticeable that the highest adsorption of Li+ at optimized parameters are in the following order: RGO/Ni3-MnO2 (63 mg g-1) > RGO/Ni2-MnO2 (56 mg g-1) > RGO/Ni1-MnO2 (52 mg g-1). A Kinetic study revealed that the experimental data were best designated pseudo-second order for each adsorbent. Li+ desorption experiments were performed using HCl as an extracting agent. Furthermore, all adsorbents exhibit efficient regeneration ability and to some extent satisfying selectivity for Li+ recovery. Briefly, it can be concluded that among the fabricated adsorbents, the RGO/Ni3-MnO2 exhibited the greatest potential for Li+ uptake from aqueous solutions as compared to others.

13.
Biomater Sci ; 7(11): 4800-4812, 2019 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-31528924

RESUMO

The reversible volume transition of redox-responsive hydrogels by near-infrared (NIR) irradiation has recently attracted significant attention as a novel therapy matrix for tracking and treating cancer via stimuli-responsive fluorescence on/off with controllable volume transition via a wireless sensing system. Herein, a NIR-induced redox-sensitive hydrogel was synthesized by blending a hydrogel with IR825-loaded carbon dots (CD) to achieve enhanced mobility of nanoparticles inside a gel network, and reversible volume phase transitions remotely controlled by a smartphone application via the induction of different redox environments. The presence of CD-IR825 in the thermosensitive poly(N-isopropylacrylamide) hydrogel network imparted fluorescence, electronic and photothermal properties to the hydrogels, which resulted in volume shrinkage behavior of the hydrogel upon exposure to NIR laser irradiation due to the redox-sensitive CDs. Under the NIR on/off cycles, the photothermal temperature, fluorescence, and porous structure were reversed after turning off the NIR laser. The hydrogel responsiveness under GSH and NIR light was studied using a wireless device based on the changes in the resistance graph on a smartphone application, generating a fast and simple method for the investigation of hydrogel properties. The in vitro cell viabilities of the MDA-MB cancer cells incubated with the composite hydrogel in the presence of external GSH exhibited a higher photothermal temperature, and the cancer cells were effectively killed after the NIR irradiation. Therefore, the NIR-induced redox-responsive nanocomposite hydrogel prepared herein has potential for use in cancer treatment and will enable the study of nanoparticle motion in hydrogel networks under multiple stimuli via a wireless device using a faster and more convenient method.


Assuntos
Resinas Acrílicas/química , Carbono/química , Hidrogéis/química , Neoplasias/terapia , Fototerapia , Pontos Quânticos/química , Temperatura , Sobrevivência Celular , Humanos , Raios Infravermelhos , Estrutura Molecular , Oxirredução , Células Tumorais Cultivadas
14.
Eur J Pharm Sci ; 134: 256-265, 2019 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-31047968

RESUMO

A redox-responsive fluorescent carbon nanogel (FCN) was designed as a bioimaging probe for targeted drug delivery to cancer cells. FCN was synthesized by the carbonization of disulfide cross-linked hyaluronic acid in the fluorescence "on" mode, followed by the attachment of manganese oxide (MnO2) nanosheets for fluorescence quenching (fluorescence "off"). We hypothesized that the fluorescence intensity of paclitaxel (PTX)-MnO2/FCN would suddenly increase (fluorescence "on") in the presence of a high level of glutathione (GSH) in cancer cells, owing to the reduction of MnO2 to Mn2+ and cleavage of the disulfide bond. Consequently, PTX would be released from the FCN system. Consistent with this hypothesis, the designed system recovered FCN fluorescence and triggered drug release through the cleavage of the disulfide bond by GSH. Moreover, PTX-MnO2/FCN demonstrated stable fluorescence intensity after GSH treatment, serving as a potential biosensor. PTX-MnO2/FCN exhibited excellent biocompatibility with normal cells and selectively targeted tumor cells, highlighting the therapeutic capabilities of this system. The developed PTX-MnO2/FCN structure may serve as a smart drug delivery system with diagnostic and therapeutic properties, good selectivity, and compatibility, and with excellent potential for biomedical applications.


Assuntos
Neoplasias da Mama/tratamento farmacológico , Sistemas de Liberação de Medicamentos/métodos , Fluorescência , Compostos de Manganês/química , Óxidos/química , Paclitaxel/administração & dosagem , Animais , Carbono/química , Linhagem Celular Tumoral/citologia , Sobrevivência Celular/efeitos dos fármacos , Cães , Liberação Controlada de Fármacos , Glutationa/farmacologia , Ácido Hialurônico/química , Células Madin Darby de Rim Canino , Nanocompostos/química , Nanopartículas , Oxirredução , Paclitaxel/farmacologia , Polímeros/química
15.
Mater Sci Eng C Mater Biol Appl ; 101: 159-168, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-31029309

RESUMO

Using pH-switchable fluorescent polymer dots (PD) by means of fluorescent, colorimetric, and electrochemical signals generated from surfaces coated with PD of zwitterionic structure provided a fast and easy method to assess their performance in mammalian cell and bacterial interactions. The PD-coated surfaces showed high sensitivity over a broad range of pH levels by switching reversibly zwitterionic states, which led to an excellent cellular resistance effect by inhibiting the attachment of nearly 95% of mammalian cells. Similarly, they exhibited a strong interaction with the negatively charged surfaces of bacteria, as observed in the fluorescence ON/OFF system. In addition, PD were employed to detect the attachment of mammalian and bacterial cells: we deposited PD on a screen-printed carbon electrode for cyclic voltammetry analysis. Notably, the presence of cells remarkably interfered with the current flow between the PD and the screen-printed carbon electrode surface by causing an impressive decline in both reduction-oxidation signals, implying the high sensitivity of the PD-coated surfaces to cells and bacteria in different pH environments. Therefore, as smart materials with high sensitivity, biocompatibility, selectivity, and accuracy, PD-coated surfaces represent a promising approach to visualizing and controlling biological cell attachment, thereby helping to avoid contamination in biomedical applications.


Assuntos
Materiais Revestidos Biocompatíveis/farmacologia , Técnicas Eletroquímicas/métodos , Escherichia coli/efeitos dos fármacos , Corantes Fluorescentes/química , Polímeros/farmacologia , Staphylococcus aureus/efeitos dos fármacos , Animais , Aderência Bacteriana/efeitos dos fármacos , Morte Celular/efeitos dos fármacos , Cães , Células HeLa , Humanos , Concentração de Íons de Hidrogênio , Interações Hidrofóbicas e Hidrofílicas , Células Madin Darby de Rim Canino , Testes de Sensibilidade Microbiana , Polímeros/química , Espectroscopia de Prótons por Ressonância Magnética , Espectrofotometria Ultravioleta , Água/química
16.
Biomater Sci ; 7(6): 2600-2610, 2019 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-30984942

RESUMO

Here, we designed a pH-responsive Indocyanine Green (ICG)-loaded zwitterion fluorescent carbon dot (CD)-encapsulating mesoporous silica nanoparticle (MSN) for pH-tunable image-guided photothermal therapy. ICG was loaded into MSN(CD) via hydrophobic and electrostatic interactions between zwitterionic CDs and ICG to achieve a controlled photothermal temperature with a fluorescent "off/on" system. The porosity of the MSNs was altered after ICG loading because of intermolecular interactions between the CDs and ICG inside the MSN shell and core, which blocked the MSN pore. The acidic environment pH affected the fluorescent signals of the ICG-MSN(CD), reflecting the "off-on" characteristics of the synthesized MSN, which then induced the release of ICG from the matrices. Moreover, the photothermal conversion of ICG-MSN(CD) showed sufficient heat generation to kill cancer cells at an acidic pH with low-temperature elevation at physiological pH. ICG-MSN(CD) demonstrated good cell viability of MDA-MB-231 cells without irradiation; however, high necrosis was observed when the environment was adjusted to acidic pH and after near-infrared irradiation. These pH-responsive photothermal mesoporous silica nanoparticles may have applications in biomedicine, particularly for cancer treatment.


Assuntos
Carbono/química , Portadores de Fármacos/química , Liberação Controlada de Fármacos , Raios Infravermelhos , Nanopartículas/química , Fototerapia , Dióxido de Silício/química , Transporte Biológico , Linhagem Celular Tumoral , Sobrevivência Celular/efeitos dos fármacos , Temperatura Alta , Humanos , Concentração de Íons de Hidrogênio , Verde de Indocianina/química , Verde de Indocianina/metabolismo , Verde de Indocianina/farmacologia , Necrose/induzido quimicamente , Porosidade , Espécies Reativas de Oxigênio/metabolismo
17.
Mater Sci Eng C Mater Biol Appl ; 97: 613-623, 2019 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-30678948

RESUMO

Innovative methods to detect and kill pathogenic bacteria have a pivotal role in the eradication of infectious diseases and the prevention of the growth of antibiotic-resistant bacteria. The combination of fluorescent carbon dots (FCDs) with silver nanoparticles (AgNPs) is an effective material for synergic detection and antimicrobial activity determination. However, the fluorescence quenching of the FCDs owing to an interaction with AgNP is a major limitation. In this study, we designed a system to utilize poly(vinylpyrrolidone) (PVP) and catechol chemistry (PVP@Ag:FCD) in order to avoid the fluorescence quenching of the FCD-AgNP combination due to Forster Resonance Energy Transfer (FRET). PVP@Ag:FCD exhibited bright fluorescence, which can be used for bacterial detection, through the promotion of electrostatic binding with the negatively-charged bacterial surface and generation of fluorescence quenching due to aggregation-induced quenching. Furthermore, the presence of silver nanoparticles in PVP@Ag:FCD produced an excellent bacteria killing efficiency against E. coli and S. aureus, even at low concentrations (0.1 mg/mL). In contaminated river water, the PVP@Ag:FCD system showed a simple, highly sensitive, and effective performance for both the detection and eradication of bacteria. Therefore, this system offers an auspicious method for the future detection and killing of bacteria.


Assuntos
Carbono/química , Nanopartículas Metálicas/química , Pontos Quânticos/química , Prata/química , Animais , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Catecóis/química , Sobrevivência Celular/efeitos dos fármacos , Cães , Escherichia coli/efeitos dos fármacos , Transferência Ressonante de Energia de Fluorescência , Células Madin Darby de Rim Canino , Nanopartículas Metálicas/toxicidade , Microscopia Confocal , Tamanho da Partícula , Povidona/química , Staphylococcus aureus/efeitos dos fármacos , Eletricidade Estática , Purificação da Água/métodos
18.
ChemMedChem ; 13(22): 2437-2447, 2018 11 20.
Artigo em Inglês | MEDLINE | ID: mdl-30288948

RESUMO

In the present study, a pH/redox-responsive cationic polymer dot (CD) was successfully prepared for a near-infrared (NIR)-mediated, simultaneously controllable photothermal temperature guided imaging off/on system to monitor therapeutic delivery. Carbonized disulfide cross-linked branched polyethyleneimine (bPEI) was conjugated with folic acid (FA) as a targeting moiety and partially formed an ionic complex with anionic indocyanine green (ICG) to afford a bPEI-based CD (ICG-CD). This was responsive to mild reductive (glutathione, GSH) and acidic tumor conditions, which enabled the simultaneous biodegradation of those hydrophobic and complex sites. The ICG-CD internalized readily into the cytoplasm of cancer cells by a FA receptor and cationic-mediated endocytosis in the off state, whereas if ICG-CD met intracellular GSH at high concentrations, GSH contributed partially to the recovery of fluorescence and was then internalized into acidic endosomes to induce complete restoration of fluorescence. This tumor-sensitive degradability of the CD not only facilitated ICG release in the tumor location but also allowed controllable photothermal therapy effects of nanoparticles under NIR irradiation, which resulted in improved cancer therapy. Taken together, the results indicate great potential in tumor targeting, intracellular imaging, and controllable therapeutic delivery through a fluorescence off/on assay under the pH/redox conditions of cancer cells.


Assuntos
Antineoplásicos/farmacologia , Corantes Fluorescentes/farmacologia , Verde de Indocianina/farmacologia , Pontos Quânticos/química , Animais , Antineoplásicos/química , Carbono/química , Linhagem Celular Tumoral , Cães , Endocitose/fisiologia , Endossomos/metabolismo , Fluorescência , Corantes Fluorescentes/química , Corantes Fluorescentes/metabolismo , Receptores de Folato com Âncoras de GPI/metabolismo , Ácido Fólico/química , Ácido Fólico/metabolismo , Glutationa/metabolismo , Humanos , Concentração de Íons de Hidrogênio , Hipertermia Induzida/métodos , Verde de Indocianina/química , Verde de Indocianina/metabolismo , Raios Infravermelhos , Células Madin Darby de Rim Canino , Oxirredução , Fototerapia/métodos , Polietilenoglicóis/química , Polietilenoglicóis/metabolismo , Polietilenoimina/química , Polietilenoimina/metabolismo , Pontos Quânticos/efeitos da radiação , Nanomedicina Teranóstica/métodos
19.
Eur J Pharm Biopharm ; 132: 200-210, 2018 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-30266668

RESUMO

Redox-responsive polymer dot (PD) were synthesized from disulfide cross-linked polymers in a carbonized process to allow quenching effects by loading of boron-dipyrromethene (BODIPY) onto the matrix. The disulfide linkage facilitated degradation of the PD system by intracellular glutathione (GSH), leading to fluorescence recovery by BODIPY and intracellular drug release. The paclitaxel release profile showed that approximately 100% of the drug escaped from the matrix in response to 10 mM GSH, whereas less than 10% was released in the absence of GSH. In vitro studies showed that quenching produced by BODIPY loading enabled visual monitoring of cancer cell death, as the quenching disappeared when BODIPY was released by GSH inside of cancer cells. The PD contain disulfide bonds representing a GSH-triggered ligand; thus, nanocarriers presented enhanced in vivo chemotherapeutic inhibition in xenograft tumor-bearing mice localized at the cancer location, guided by fluorescent off-on system tracking and measured by the release of BODIPY. This platform reacts to the redox level in sensitive manner and cancer cell death can be monitored by fluorescence, making this platform useful for bio-applications, particularly in vitro and in vivo therapy and diagnosis, while considering the cell physiological environment. This system may be useful for wider medical applications.


Assuntos
Antineoplásicos Fitogênicos/administração & dosagem , Neoplasias/tratamento farmacológico , Paclitaxel/administração & dosagem , Polímeros/química , Animais , Antineoplásicos Fitogênicos/química , Antineoplásicos Fitogênicos/farmacologia , Compostos de Boro/química , Linhagem Celular Tumoral , Cães , Portadores de Fármacos/química , Liberação Controlada de Fármacos , Transferência Ressonante de Energia de Fluorescência/métodos , Glutationa/metabolismo , Humanos , Células Madin Darby de Rim Canino , Camundongos , Camundongos Endogâmicos BALB C , Nanopartículas , Oxirredução , Paclitaxel/química , Paclitaxel/farmacologia , Ensaios Antitumorais Modelo de Xenoenxerto
20.
J Pharm Biomed Anal ; 159: 1-10, 2018 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-29960038

RESUMO

Boronic acid, which can bind chemo-selectively and reversibly to diols, could be used for the early detection of bacteria through its affinity-binding reaction with diol groups on the bacterial cell wall. Herein, we describe the use of a diol-modified fluorescent probe (DYE) conjugated to a nanosensor consisting of phenylboronic acid-functionalized fluorescent carbon dot (FCD) to allow quenching via the Förster resonance energy transfer (FRET) process. Phenylboronic acid is well-known for its preferential affinity for diol-containing molecules through cyclic ester bond formation. Therefore, in the presence of glucose-containing bacteria, the DYE in the cyclic ester form will be released from the FCD and replaced by the bacterial cell forming a new cyclic boronate ester bond with the nanoparticle, inducing recovery of the fluorescence. Quantitatively, the system's detection performance at various bacterial concentrations (101-107 CFU/mL) reached ∼100% after 60 min, indicating that the high binding affinity of the diol moeity on the peptidoglycan (sugar)-rich bacteria was enough to displace the DYE from the boronic acid-functionalized FCD platform. Our facile and tunable fluorescence switch-on system was tested for its ability to detect bacteria in water from a contaminated river. Incredibly, the system was most successful in detecting bacteria in the contaminated river water, thus proving it to be a less expensive and more robust affinity biosensor for the detection of contaminating pathogens in various chemoselective ligand-based environments.


Assuntos
Técnicas Biossensoriais/métodos , Ácidos Borônicos/química , Escherichia coli , Corantes Fluorescentes/química , Luminescência , Staphylococcus aureus , Carbono/química , Escherichia coli/isolamento & purificação , Staphylococcus aureus/isolamento & purificação , Fatores de Tempo
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