Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 82
Filtrar
Mais filtros










Base de dados
Intervalo de ano de publicação
1.
Angew Chem Int Ed Engl ; : e202403618, 2024 May 31.
Artigo em Inglês | MEDLINE | ID: mdl-38819600

RESUMO

The sulfur reduction reaction (SRR) is an attractive 16-electron transfer process that endows Li-S batteries with a theoretical capacity of 1,672 mAh g-1. However, the slow kinetics and complex pathways of the SRR cause the shuttling of soluble polysulfides (PSs), thus fast capacity fading. Here, we report using cisplatin (cis-Pt) as a novel mediator to improve the SRR kinetics and a molecular probe to identify the SRR pathways. We show that cis-Pt with a reductive Pt2+ center can directly slice the S-S bonds of PSs, leading to enhanced charge transfer kinetics, guided SRR pathways, and depth conversion of PSs to Li2S. With cis-Pt added, Li-S coin cells deliver a maximum specific capacity of 1,437 mAh g-1 and a capacity decay of 0.017% per cycle after 1000 cycles, while a pouch cell with a practical electrolyte-sulfur ratio (2.5 µl mg-1) exhibits a high energy density of 318.8 Wh kg-1. Our mechanistic studies reveal that cis-Pt steers the cathodic SRR pathways by generating redox active cis-Pt/PSs complexes, enabling the replacement of the sluggish SRR with a faster redox cycling of Pt4+/Pt2+ pairs. These findings provide insights into the rational design of functional mediators for tackling the cathodic challenges inside Li-S batteries.

2.
Talanta ; 277: 126275, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38810380

RESUMO

The integration of smartphones with conventional analytical approaches plays a crucial role in enhancing on-site detection platforms for point-of-care testing. Here, we developed a simple, rapid, and efficient three-channel colorimetric sensor array, leveraging the peroxidase (POD)-like activity of polydopamine-decorated FeNi foam (PDFeNi foam), to identify antioxidants using both microplate readers and smartphones for signal readouts. The exceptional catalytic capacity of PDFeNi foam enabled the quick catalytic oxidation of three typical peroxidase substrates (TMB, OPD and 4-AT) within 3 min. Consequently, we constructed a colorimetric sensor array with cross-reactive responses, which was successfully applied to differentiate five antioxidants (i.e., glycine (GLY), glutathione (GSH), citric acid (CA), ascorbic acid (AA), and tannic acid (TAN)) within the concentration range of 0.1-10 µM, quantitatively analyze individual antioxidants (with AA and CA as model analytes), and assess binary mixtures of AA and GSH. The practical application was further validated by discriminating antioxidants in serum samples with a smartphone for signal readout. In addition, since pesticides could be absorbed on the surface of PDFeNi foam through π-π stacking and hydrogen bonding, the active sites were differentially masked, leading to featured modulation on POD-like activity of PDFeNi foam, thereby forming the basis for pesticides discrimination on the sensor array. The nanozyme-based sensor array provides a simple, rapid, visual and high-throughput strategy for precise identification of various analytes with a versatile platform, highlighting its potential application in point-care-of diagnostic, food safety and environmental surveillance.

3.
ACS Nano ; 18(13): 9645-9655, 2024 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-38501440

RESUMO

The utilization of alkyl radicals (•R) for hypoxic tumor therapy has great prospects due to its O2-independence and high reactivity. However, correlational initiators for in vivo activation remain scarce. Here, we report that ultrasound excitation of oleic acid-capped BaTiO3 (OA@BaTiO3) can result in an •R cascade and hence a means to conquer hypoxic tumors. Mechanistic studies find that the •R signal disappears when OA@BaTiO3 undergoes acid washing post-treatment, which is a common procedure for removing the unwanted byproduct BaCO3. Combined with the infrared spectrum analysis, acid treatment was proven to weaken the peaks at 2840-2970 cm-1 characteristic of -CH2- and terminal -CH3 stretching vibration of OA. There is compelling evidence that high temperature thermal oxidation of OA involves the generation of •R. Thus, acid washing is considered to remove the loosely bound yet catalytically active OA. And piezoelectric BaTiO3, a potential electron-hole redox catalyst, can sensitize these OA molecules and disintegrate them to •R. This unexpected discovery provides us with a distinctive mentality to seek diverse •R initiators for tumor ablation, as well as an additional perspective on the postprocessing of synthetic materials.

4.
Adv Healthc Mater ; 13(15): e2400325, 2024 06.
Artigo em Inglês | MEDLINE | ID: mdl-38364772

RESUMO

Nanozymes show great potential in facilitating tumor ferroptosis by upregulation of reactive oxygen species (ROS) and downregulation of glutathione (GSH). However, mild acidity (pH 6.5-6.9) of tumor microenvironment severely restricts the activity of nanozymes. Although lysosomes as acidic organelles (pH = 3.5-5.5) are hopeful for improving enzyme-like activity, most reported nanozymes are not capable of effectively accumulating in the lysosomes. Herein, an acid-responsive self-assembly strategy based on iron phthalocyanine-rich covalent organic framework nanosheets (COFFePc NSs) is developed, which enables lysosomal targeting aggregation of COFFePc NSs due to the existence of abundant negative hydroxyl groups and rigid structure. Meanwhile, COFFePc NSs display exceptional multienzyme-mimic performance at lower pH to efficiently generate ROS to cause lysosome damage and apoptosis by synergistic photothermal effect. Subsequently, the released COFFePc with GSH oxidase-mimicking activity can consume GSH to promote ferroptosis. This is the first report of a 2D COF using its own properties to achieve lysosomal self-assembly. Overall, the work provides a new paradigm for the development of lysosome-targeted nanosystems.


Assuntos
Ferroptose , Indóis , Isoindóis , Lisossomos , Espécies Reativas de Oxigênio , Ferroptose/efeitos dos fármacos , Lisossomos/metabolismo , Indóis/química , Indóis/farmacologia , Humanos , Espécies Reativas de Oxigênio/metabolismo , Glutationa/metabolismo , Glutationa/química , Linhagem Celular Tumoral , Animais , Estruturas Metalorgânicas/química , Estruturas Metalorgânicas/farmacologia , Camundongos
5.
J Colloid Interface Sci ; 662: 48-57, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38335739

RESUMO

Presently, most fluorescent probes for amino acid enantiomers detection require metal ions participation, which greatly increases the detection steps and costs, and affects the accuracy of detection results. To solve this problem, a dual pattern recognition sensor of chiral carbon dots (L-Try-Thr-CDs) with a quantum yield of 36.23 % was prepared by a one-step solvothermal method for the highly selective detection of lysine (Lys) enantiomers. Under optimal experimental conditions, the fluorescence and circular dichroism (CD) signals of the obtained L-Try-Thr-CDs could rapidly and effectively responded to L-Lys with limits of detection (LOD) of 16.51 nM and 24.38 nM, respectively, much lower than previously reported sensors. Importantly, the L-Try-Thr-CDs as a dual-mode sensor could not only detect amino acid enantiomers and simplify the steps, but also avoid inaccurate detection results due to unstable metal ions. Furthermore, the L-Try-Thr-CDs could detect L-Lys in living cells via a fluorescence microscope because of their excellent fluorescence characteristics and low toxicity. These results indicated that the dual-mode sensor not only provided a practical strategy for the design of new fluorescent probes, but also possessed outstanding application prospects in the accurate detection of lysine enantiomers.


Assuntos
Pontos Quânticos , Pontos Quânticos/química , Corantes Fluorescentes/química , Triptofano , Lisina , Carbono/química , Treonina , Estereoisomerismo , Íons , Espectrometria de Fluorescência
6.
J Mater Chem B ; 12(10): 2537-2546, 2024 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-38345306

RESUMO

Disulfiram (DSF), a new potential anticancer drug, has been shown to exhibit anticancer activity dependent on the formation of CuET, the chelation product of DSF with Cu2+. However, the poor stability of DSF and insufficient physiological concentration of Cu2+ hinder its practical application. To achieve the co-delivery of DSF and Cu2+ while overcoming the inefficiency of single chemotherapy, in this study, a cascade nanoplatform, DSF/Ce6@ZIF-8@CuO2, was constructed by encapsulating DSF and chlorin e6 (Ce6, a photosensitizer) in zeolite imidazole framework-8 (ZIF-8, a nanocarrier) and then loading CuO2, which self-supplied H2O2/O2, onto DSF/Ce6@ZIF-8. By triggering the response of DSF/Ce6@ZIF-8@CuO2 to the acidic tumor microenvironment, encapsulated DSF, Ce6 and CuO2 were released to achieve multimodal synergistic treatment with enhanced DSF chemotherapy and chemodynamic/photodynamic therapy (CDT/PDT). In vitro and animal studies indicated that the designed DSF/Ce6@ZIF-8@CuO2 has strong tumor-inhibitory effects and provides a promising paradigm for designing smart nanoplatforms.


Assuntos
Neoplasias , Fotoquimioterapia , Animais , Microambiente Tumoral , Peróxido de Hidrogênio/farmacologia , Fármacos Fotossensibilizantes/farmacologia , Fármacos Fotossensibilizantes/uso terapêutico , Neoplasias/tratamento farmacológico
7.
Small ; 20(22): e2309501, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38109067

RESUMO

The development of lithium-based solid-state batteries (SSBs) has to date been hindered by the limited ionic conductivity of solid polymer electrolytes (SPEs), where nonsolvated Li-ions are difficult to migrate in a polymer framework at room temperature. Despite the improved cationic migration by traditional heating systems, they are far from practical applications of SSBs. Here, an innovative strategy of light-mediated energy conversion is reported to build photothermal-based SPEs (PT-SPEs). The results suggest that the nanostructured photothermal materials acting as a powerful light-to-heat converter enable heating within a submicron space, leading to a decreased Li+ migration barrier and a stronger solid electrolyte interface. Via in situ X-ray diffraction analysis and molecular dynamics simulation, it is shown that the generated heating effectively triggers the structural transition of SPEs from a highly crystalline to an amorphous state, that helps mediate lithium-ion transport. Using the assembled SSBs for exemplification, PT-SPEs function as efficient ion-transport media, providing outstanding capacity retention (96% after 150 cycles) and a stable charge/discharge capacity (140 mA g-1 at 1.0 C). Overall, the work provides a comprehensive picture of the Li-ion transport in solid polymer electrolytes and suggests that free volume may be critical to achieving high-performance solid-state batteries.

8.
ACS Appl Mater Interfaces ; 15(36): 42532-42540, 2023 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-37646500

RESUMO

Machine learning (ML) coupled with quantum chemistry calculations predicts catalyst properties with high accuracy; however, ML approaches in the design of multicomponent catalysts primarily rely on simulation data because obtaining sufficient experimental data in a short time is difficult. Herein, we developed a rapid screening strategy involving nanodroplet-mediated electrodeposition using a carbon nanocorn electrode as the support substrate that enables complete data collection for training artificial intelligence networks in one week. The inert support substrate ensures intrinsic activity measurement and operando characterization of the irreversible reconstruction of multinary alloy particles during the oxygen evolution reaction. Our approach works as a closed loop: catalyst synthesis-in situ measurement and characterization-database construction-ML analysis-catalyst design. Using artificial neural networks, the ML analysis revealed that the entropy values of multicomponent catalysts are proportional to their catalytic activity. The catalytic activities of high-entropy systems with different components varied little, and the overall catalytic activity was greater than that of the medium-low-entropy system. These findings will serve as a guideline for the design of catalysts.

9.
Adv Mater ; 35(44): e2304120, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37467076

RESUMO

Sluggish kinetics and parasitic shuttling reactions severely impede lithium-sulfur (Li-S) battery operation; resolving these issues can enhance the capacity retention and cyclability of Li-S cells. Therefore, an effective strategy featuring core-shell-structured Co/Ni bimetal-doped metal-organic framework (MOF)/sulfur nanoparticles is reported herein for addressing these problems; this approach offers unprecedented spatial confinement and abundant catalytic sites by encapsulating sulfur within an ordered architecture. The protective shells exhibit long-term stability, ion screening, high lithium-polysulfide adsorption capability, and decent multistep catalytic conversion. Additionally, the delocalized electrons of the MOF endow the cathodes with superior electron/lithium-ion transfer ability. Via multiple physicochemical and theoretical analysis, the resulting synergistic interactions are proved to significantly promote interfacial charge-transfer kinetics, facilitate sulfur conversion dynamics, and inhibit shuttling. The assembled Li-S batteries deliver a stable, highly reversible capacity with marginal decay (0.075% per cycle) for 400 cycles at 0.2 C, a pouch-cell areal capacity of 3.8 mAh cm-2 for 200 cycles under a high sulfur loading, as well as remarkably improved pouch-cell performance.

10.
Adv Healthc Mater ; 12(28): e2301502, 2023 11.
Artigo em Inglês | MEDLINE | ID: mdl-37409492

RESUMO

Hydroxyl radical (• OH) as a highly oxidizing reactive oxygen species can induce immunogenic cell death (ICD) in cancer treatment. However, high-efficiency cancer immunotherapy is still a huge challenge due to the low • OH generation efficiency in the tumor microenvironment, resulting in insufficient immunogenicity and the poor immune response. Here, a near-infrared (NIR) light-enhanced • OH generation strategy is developed for cancer immunotherapy by using a copper-based metal-organic framework (Cu-DBC) nanoplatform. With this strategy, the generation efficiency of • OH under NIR irradiation is increased 7.34 times than that without NIR irradiation, which induces robust ICD and immune response, thus leading to primary tumor elimination and the inhibition of distant tumor growth and tumor lung metastasis. Experimental results show that Cu-DBC can induce • OH boosting through photothermal (PT)-enhanced Cu-catalytic Fenton-like reaction and photocatalytic electron transfer under NIR light irradiation to amplify tumor ICD for immunotherapy.


Assuntos
Nanopartículas , Neoplasias , Humanos , Radical Hidroxila , Cobre/farmacologia , Raios Infravermelhos , Neoplasias/terapia , Imunoterapia/métodos , Linhagem Celular Tumoral , Microambiente Tumoral
11.
Small Methods ; 7(10): e2300523, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37452519

RESUMO

Lithium-sulfur batteries (LSBs) as a next-generation promising energy storage device have a great potential commercial application due to their high specific capacity and energy density. However, it is still a challenge to real-time monitor the evolution process of polysulfides during the LSBs discharge process. Herein, an in situ electrochemical-fluorescence technology is developed to measure the fluorescence intensity change of cadmium sulfide quantum dots (CdS QDs) during the LSBs discharge process in real-time, which could monitor the evolution process of polysulfides. First, the real-time fluorescent spectrum and confocal fluorescence imaging of discharge processes for LSBs with CdS QDs are integrally illustrated. Furthermore, the fluorescence spectra and imaging results show that CdS QDs could immobilize polysulfides through bonding with polysulfides to improve the LSB device performance. This in situ electrochemical-fluorescence technology provides a new in situ and real-time-monitor method for better understanding the working mechanism of LSBs.

12.
J Mater Chem B ; 11(13): 2886-2894, 2023 03 30.
Artigo em Inglês | MEDLINE | ID: mdl-36942660

RESUMO

Calcination has been widely demonstrated as a favorable protocol for producing various inorganic nanomaterials for tumor therapy. However, little attention has been paid to its effect on the biotherapeutic efficacy of inorganic nanomaterials. Herein, we compare the effects of different calcination atmospheres on the therapeutic efficacy of Fe-V-O (FVO) nanomaterials. We find that compared with FVO nanomaterials synthesized by calcination in air, those prepared by argon calcination have a lower metallic valence state and a higher near-infrared light absorption capacity, hence resulting in significantly better biosafety and higher chemodynamic therapy (CDT)/photothermal therapy (PTT) efficacy. This study demonstrates that the therapeutic efficacy of inorganic nanomaterials can be optimized by employing different thermal treatment atmospheres, which provides new insights into the development of efficient anti-tumor agents.


Assuntos
Nanopartículas , Fototerapia , Fototerapia/métodos , Vanádio , Nanopartículas/uso terapêutico , Óxidos , Ferro
13.
Angew Chem Int Ed Engl ; 62(19): e202216822, 2023 05 02.
Artigo em Inglês | MEDLINE | ID: mdl-36917027

RESUMO

Pd-catalyzed chemistry has played a significant role in the growing subfield of bioorthogonal catalysis. However, rationally designing Pd nanocatalysts that show outstanding catalytic activity and good biocompatibility poses a great challenge. Herein, we propose an innovative strategy through exploiting black phosphorous nanosheets (BPNSs) to enhance Pd-mediated bioorthogonal catalytic activity. Firstly, the electron-donor properties of BPNSs enable in situ growth of Pd nanoparticles (PdNPs) on it. Meanwhile, due to the superb capability of reducing PdII , BPNSs can act as hard nucleophiles to accelerate the transmetallation in the decaging reaction process. Secondly, the lone pair electrons of BPNSs can firmly anchor PdNPs on their surface via Pd-P bonds. This design endows Pd/BP with the capability to retard tumor growth by activating prodrugs. This work proposes new insights into the design of heterogeneous transition-metal catalysts (TMCs) for bioorthogonal catalysis.


Assuntos
Nanopartículas , Neoplasias , Pró-Fármacos , Humanos , Paládio/química , Fósforo , Neoplasias/patologia , Catálise
14.
Acta Biomater ; 158: 625-636, 2023 03 01.
Artigo em Inglês | MEDLINE | ID: mdl-36608895

RESUMO

The antioxidant system of tumor cells severely impairs reactive oxygen species (ROS)-mediated tumor therapy. Despite extensive attempts to attenuate the antioxidant capacity by eliminating ROS scavengers such as glutathione (GSH), nicotinamide adenine dinucleotide phosphate (NADPH) over-expressed in the tumor microenvironment can regenerate GSH from glutathione disulfide (GSSG), hence weakening ROS-induced oxidative damage. Therefore, engineering a nanoplatform capable of depleting both NADPH and GSH is extremely significant for improving ROS-mediated tumor treatment. Herein, a synergetic antioxidant inhibition strategy is proposed to attenuate intracellular antioxidant capacity for hypoxic tumor therapy. In this context, both porous Prussian blue nanoparticles (PPB NPs) and cisplatin prodrug [cis-Pt (IV)] in the nanoplatform can oxidize GSH to directly reduce GSH levels, while PPB NPs also enable NADPH depletion by peroxidase-mimicking to impair GSH regeneration. Furthermore, PPB NPs with catalase-mimicking activity catalyze H2O2 decomposition to alleviate tumor hypoxia, thus reducing the generation of GSH and boosting singlet oxygen (1O2) production by Chlorin e6 (Ce6) for enhancing oxidative damage. Experimental results prove that the nanoplatform, denoted as PPB-Ce6-Pt, can induce remarkable tumor cells apoptosis and ferroptosis. Importantly, a simple loading method and the use of Food Drug Administration (FDA)-approved materials make PPB-Ce6-Pt have great potential for practical applications. STATEMENT OF SIGNIFICANCE: The antioxidant system in tumor cells disables ROS-mediated tumor therapy. Besides, extensive attempts aim at depleting GSH without considering their regeneration. Therefore, we developed a synergetic strategy to attenuate intracellular antioxidant capacity for hypoxic tumor therapy. PPB-Ce6-Pt nanoplatform could not only directly reduce GSH levels but also deplete NADPH by peroxidase-mimicking to impair GSH regeneration. In addition, PPB-Ce6-Pt nanoplatform could catalyze H2O2 decomposition to alleviate tumor hypoxia, thus reducing the generation of GSH and boosting 1O2 production by Chlorin e6 (Ce6) for increasing oxidative damage. Then, intracellular ROS boost and redox dyshomeostasis induced remarkable tumor cells apoptosis and ferroptosis. Importantly, a simple loading method and the use of biosafety materials made the nanoplatform have great potential for practical applications.


Assuntos
Nanopartículas , Neoplasias , Fotoquimioterapia , Humanos , Antioxidantes/farmacologia , Fotoquimioterapia/métodos , Espécies Reativas de Oxigênio , Peróxido de Hidrogênio/química , NADP/farmacologia , NADP/uso terapêutico , Estresse Oxidativo , Neoplasias/tratamento farmacológico , Glutationa/metabolismo , Nanopartículas/química , Peroxidases/farmacologia , Peroxidases/uso terapêutico , Linhagem Celular Tumoral , Fármacos Fotossensibilizantes/química , Microambiente Tumoral
15.
ACS Appl Mater Interfaces ; 15(1): 524-540, 2023 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-36542560

RESUMO

Current therapeutic strategies for Alzheimer's disease (AD) mainly focus on inhibition of aberrant amyloid-ß peptide (Aß) aggregation. However, these strategies cannot repair the side symptoms (e.g., high neuronal oxidative stress) triggered by Aß accumulation and thus show limited effects on suppressing Aß-induced neuronal apoptosis. Herein, we develop a stepwise metal-phenolic coordination approach for the rational design of a neuroprotection enhancer, K8@Fe-Rh/Pda NPs, in which rhein and polydopamine are effectively coupled to enhance the treatment of AD in APPswe/PSEN1dE9 transgenic (APP/PS1) mice. We discover that the polydopamine inhibits the aggregation of Aß oligomers, and rhein helps repair damage to neurons triggered by Aß aggregation. Based on molecular docking, we demonstrate that the polydopamine has a strong interaction with Aß monomers/fibrils through its multiple recognition sites (e.g., catechol groups, imine groups, and indolic/catecholic π-systems), thereby reducing Aß burden. Further investigation of the antioxidant mechanisms suggests that K8@Fe-Rh/Pda NPs promote the mitochondrial biogenesis via activating the sirtuin 1 (SIRT1)/peroxisome proliferator-activated receptor gamma coactivator 1-alpha pathway. This finally inhibits neuronal apoptosis. Moreover, an intravenous injection of these nanoparticles potently improves the cognitive function in APP/PS1 mice without adverse effects. Overall, our work provides a promising approach to develop advanced nanomaterials for multi-target treatment of AD.


Assuntos
Doença de Alzheimer , Nanopartículas , Camundongos , Animais , Doença de Alzheimer/tratamento farmacológico , Doença de Alzheimer/metabolismo , Simulação de Acoplamento Molecular , Neuroproteção , Camundongos Transgênicos , Peptídeos beta-Amiloides/metabolismo , Modelos Animais de Doenças
16.
Biosens Bioelectron ; 216: 114667, 2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-36099836

RESUMO

Biosensors is an advanced detection and monitoring device for the development of biotechnology, and is also a rapid and microanalytical device at the molecular level. Demands for high sensitivity, high flexibility, good biocompatibility, easy chemical modification and low cost offer incentive for exploring new materials to develop the next-generation biosensors. With the vigorous development of organic electronics, the performances of organic devices have been effectively improved, leading to organic semiconductor materials with low cost, good flexibility, easy chemical modification and good biocompatibility for biosensors. Biosensors based on organic field-effect transistors (OFETs) have become one of the most advanced biosensor platforms because of their inherent ability to amplify received signals. Furthermore, OFET-based biosensors have been widely used in the detection of DNA, protein, cell, glucose and other biological substances due to its high sensitivity, fast analysis speed, label-free detection, small size and simple operation. This mini review briefly discusses the organic small molecule semiconductor materials, device configurations, basic principles and application fields of OFETs-based biosensors.


Assuntos
Técnicas Biossensoriais , Transistores Eletrônicos , DNA , Glucose , Semicondutores
17.
Biomater Sci ; 10(20): 5947-5955, 2022 Oct 11.
Artigo em Inglês | MEDLINE | ID: mdl-36043518

RESUMO

Mitigating cellular resistance, which could enhance the sensitivity of tumor cells to treatment, is a promising approach for obtaining better therapeutic outcomes. However, the present designs of materials generally disregard this point, or only focus on a single specific resistance. Herein, a strategy based on a series of cascade reactions aiming to suppress multiple cellular resistances is designed by integrating photothermal and chemotherapy into a mitochondria targeted nanosystem (AuBPs@TD). The intelligent nanosystem is fabricated by modifying gold nanobipyramids (AuBPs) with triphenylphosphonium (TPP) functionalized dichloroacetic acid (DCA). TPP serves as a "navigation system" and facilitates the location of AuBPs@TD in the mitochondria. Moreover, the released DCA promoted by the photothermal effect of AuBPs, as the mitochondrial kinase inhibitor, could inhibit glycolysis, and lead to a repressed expression of heat shock protein 90, which is the main resistance protein in cancer cells against photothermal therapy (PTT). Thus, the photothermal antitumor effect can be significantly improved. For the other cascade passage, the hyperthermal atmosphere depresses the expression of P-glycoprotein, a protein associated with drug resistance, and consequently prevents DCA molecules from being expelled in return. Furthermore, the retained DCA molecules elevate the concentration of intracellular hydrogen peroxide, and due to the peroxidase-like activity of AuBPs, increased intracellular reactive oxygen species could be obtained to accelerate apoptosis. As a result, these cascade reactions lead to significant inhibition of cellular resistance and greatly improve the therapeutic performance. This work paves a new way for suppressing cellular resistance to achieve the desired therapeutic effect.


Assuntos
Ácido Dicloroacético , Peróxido de Hidrogênio , Subfamília B de Transportador de Cassetes de Ligação de ATP , Linhagem Celular Tumoral , Ácido Dicloroacético/farmacologia , Ouro/metabolismo , Proteínas de Choque Térmico/metabolismo , Proteínas de Choque Térmico/farmacologia , Peróxido de Hidrogênio/metabolismo , Mitocôndrias , Peroxidases/metabolismo , Peroxidases/farmacologia , Espécies Reativas de Oxigênio/metabolismo
18.
J Mater Chem B ; 10(22): 4261-4273, 2022 06 08.
Artigo em Inglês | MEDLINE | ID: mdl-35583206

RESUMO

Micelles as nanocarriers not only offer new opportunities for early diagnosis and treatment of malignant cancers but also encounter numerous barriers in the path of efficient delivery of drugs to diseased areas in the body. To address these issues, we developed a pH/GSH responsive nano-prodrug micelle (NLG919/PGA-Cys-PPA@Gd) with a high drug-loading ratio and controlled drug release performance for MRI-guided tumor photodynamic therapy (PDT) and immune synergistic therapy. Under normal conditions, theranostic nanomicelles remained stable and in a photo-quenched state. Upon accumulation in the tumor site, however, the micelles demonstrated tumor microenvironment (TME) triggered photoactive formed-PPA (a photosensitizer) and NLG919 (an indoleamine 2,3-dioxygenase (IDO) inhibitor) release because the amide bonds of PGA-Cys-PPA and the disulfide linkage of Cys were sensitive to pH and GSH, respectively. More importantly, these micelles could avoid the undesired PPA leakage in blood circulation due to the conjugation between PPA and polymers. Furthermore, the obtained micelles could also enhance the contrast of T1-weighted MRI of tumors by virtue of their high relaxivity (r1 = 29.85 mM-1 s-1). In vitro and in vivo results illustrated that the micelles had good biocompatibility and biosafety. On the basis of the efficient drug delivery strategies in PDT and IDO pathway inhibition, this intelligent dual-drug delivery system could serve as an effective approach for MRI guided combination therapy of cancer.


Assuntos
Neoplasias , Fotoquimioterapia , Pró-Fármacos , Humanos , Imageamento por Ressonância Magnética , Micelas , Neoplasias/diagnóstico por imagem , Neoplasias/tratamento farmacológico , Pró-Fármacos/química , Triazenos , Microambiente Tumoral
19.
J Colloid Interface Sci ; 609: 279-288, 2022 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-34902671

RESUMO

Room temperature phosphorescence (RTP) materials have been widely noticed due to their superior optical properties in the past decade. Herein, we report the Si-assisted N, P co-doped RTP carbonized polymer dots (CPDs), prepared by one-step microwave assisted heating of 3-(2-Aminoethylamino)propyldimethoxymethylsilane and phosphoric acid aqueous solution. The obtained CPDs exhibit bright RTP with an absolute photoluminescence quantum yield 34.17%, absolute phosphorescence quantum yield 11.42% and long lifetime of 1.42 s, which lasts for about 16 s to the naked eyes. We apply the obtained CPDs into information encryption and Polyethyleneterephthalate (PET) film graphic anti-counterfeiting with facile way. Additionally, we make more efforts to realize aqueous RTP CPDs composite. The obtained aqueous CPDs composite exhibits bright aqueous RTP with absolute photoluminescence quantum yield (QY) of 12.61%, absolute phosphorescence quantum yield (QY) of 5.08% and RTP lifetime of 1.46 s, which lasts for about 10 s to the naked eyes. The RTP CPDs composite is nontoxic and biocompatible. These brilliant characteristics allow CPDs composite to be applicable in biological imaging. Thisstudy affords a new RTP material which can be easily prepared and used for information encryption, graphic anti-counterfeiting and biological imaging.


Assuntos
Polímeros , Pontos Quânticos , Diagnóstico por Imagem , Temperatura
20.
ACS Appl Mater Interfaces ; 13(30): 35568-35578, 2021 Aug 04.
Artigo em Inglês | MEDLINE | ID: mdl-34286585

RESUMO

Mitochondria-targeted synergistic therapy, including photothermal (PTT) and photodynamic therapy (PDT), has aroused wide attention due to the high sensitivity to reactive oxygen species (ROS) and heat shock of mitochondria. However, most of the developed nanosystems for the combinatorial functions require the integration of different components, such as photosensitizers and mitochondria-targeted molecules. Consequently, it indispensably requires sophisticated design and complex synthetic procedures. In this work, a well-designed Bi2S3-based nanoneedle, that localizes to mitochondria and produces extra ROS with inherent photothermal effect, was reported by doping of Fe (denoted as FeBS). The engineered intrinsic characteristics certify the capacity of such "one-for-all" nanosystems without additional molecules. The lipophilicity and surface positive charge are demonstrated as crucial factors for specifical mitochondria targeting. Significantly, Fe doping overcomes the disadvantage of the narrow band gap of Bi2S3 to prevent the fast recombination of electron-hole, hence resulting in the generation of ROS for PDT. The "one-for-all" nanoparticles integrate with mitochondria-targeting and synergistic effect of PDT and PTT, thus exhibit enhanced therapeutic effect and inhibit the growth of tumors observably. This strategy may open a new direction in designing the mitochondria-targeted materials and broadening the properties of inorganic semiconductor materials for satisfactory therapeutic outcomes.


Assuntos
Antineoplásicos/uso terapêutico , Mitocôndrias/efeitos dos fármacos , Nanopartículas/química , Neoplasias/tratamento farmacológico , Fármacos Fotossensibilizantes/uso terapêutico , Animais , Antineoplásicos/farmacologia , Antineoplásicos/toxicidade , Bismuto/química , Feminino , Células HeLa , Humanos , Ferro/química , Camundongos Endogâmicos BALB C , Fotoquimioterapia , Fármacos Fotossensibilizantes/farmacologia , Fármacos Fotossensibilizantes/toxicidade , Terapia Fototérmica , Espécies Reativas de Oxigênio/metabolismo , Sulfetos/química
SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA
...