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1.
ACS Nano ; 18(19): 12477-12488, 2024 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-38699877

RESUMO

Progress in the design and synthesis of nanostructured self-assembling systems has facilitated the realization of numerous nanoscale geometries, including fibers, ribbons, and sheets. A key challenge has been achieving control across multiple length scales and creating macroscopic structures with nanoscale organization. Here, we present a facile extrusion-based fabrication method to produce anisotropic, nanofibrous hydrogels using self-assembling peptides. The application of shear force coinciding with ion-triggered gelation is used to kinetically trap supramolecular nanofibers into aligned, hierarchical macrostructures. Further, we demonstrate the ability to tune the nanostructure of macroscopic hydrogels through modulating phosphate buffer concentration during peptide self-assembly. In addition, increases in the nanostructural anisotropy of fabricated hydrogels are found to enhance their strength and stiffness under hydrated conditions. To demonstrate their utility as an extracellular matrix-mimetic biomaterial, aligned nanofibrous hydrogels are used to guide directional spreading of multiple cell types, but strikingly, increased matrix alignment is not always correlated with increased cellular alignment. Nanoscale observations reveal differences in cell-matrix interactions between variably aligned scaffolds and implicate the need for mechanical coupling for cells to understand nanofibrous alignment cues. In total, innovations in the supramolecular engineering of self-assembling peptides allow us to decouple nanostructure from macrostructure and generate a gradient of anisotropic nanofibrous hydrogels. We anticipate that control of architecture at multiple length scales will be critical for a variety of applications, including the bottom-up tissue engineering explored here.


Assuntos
Hidrogéis , Nanofibras , Peptídeos , Nanofibras/química , Peptídeos/química , Hidrogéis/química , Humanos , Materiais Biocompatíveis/química , Materiais Biocompatíveis/síntese química , Anisotropia , Animais
2.
J Am Chem Soc ; 146(20): 13903-13913, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38721817

RESUMO

Cohesive and interfacial adhesion energies are difficult to balance to obtain reversible adhesives with both high mechanical strength and high adhesion strength, although various methods have been extensively investigated. Here, a biocompatible citric acid/L-(-)-carnitine (CAC)-based ionic liquid was developed as a solvent to prepare tough and high adhesion strength ionogels for reversible engineered and biological adhesives. The prepared ionogels exhibited good mechanical properties, including tensile strength (14.4 MPa), Young's modulus (48.1 MPa), toughness (115.2 MJ m-3), and high adhesion strength on the glass substrate (24.4 MPa). Furthermore, the ionogels can form mechanically matched tough adhesion at the interface of wet biological tissues (interfacial toughness about 191 J m-2) and can be detached by saline solution on demand, thus extending potential applications in various clinical scenarios such as wound adhesion and nondestructive transfer of organs.


Assuntos
Materiais Biocompatíveis , Ácido Cítrico , Géis , Materiais Biocompatíveis/química , Materiais Biocompatíveis/síntese química , Ácido Cítrico/química , Géis/química , Carnitina/química , Líquidos Iônicos/química , Resistência à Tração , Adesivos/química
3.
ACS Appl Bio Mater ; 7(5): 3154-3163, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38695332

RESUMO

ß-Galactosidase (ß-Gala) is an essential biomarker enzyme for early detection of breast tumors and cellular senescence. Creating an accurate way to monitor ß-Gala activity is critical for biological research and early cancer detection. This work used fluorometric, colorimetric, and paper-based color sensing approaches to determine ß-Gala activity effectively. Via the sensing performance, the catalytic activity of ß-Gala resulted in silicon nanoparticles (SiNPs), fluorescent indicators obtained via a one-pot hydrothermal process. As a standard enzymatic hydrolysis product of the substrate, kaempferol 3-O-ß-d-galactopyranoside (KOßDG) caused the fluorometric signal to be attenuated on kaempferol-silicon nanoparticles (K-SiNPs). The sensing methods demonstrated a satisfactory linear response in sensing ß-Gala and a low detection limit. The findings showed the low limit of detection (LOD) as 0.00057 and 0.098 U/mL for fluorometric and colorimetric, respectively. The designed probe was then used to evaluate the catalytic activity of ß-Gala in yogurt and human serum, with recoveries ranging from 98.33 to 107.9%. The designed sensing approach was also applied to biological sample analysis. In contrast, breast cancer cells (MCF-7) were used as a model to test the in vitro toxicity and molecular fluorescence imaging potential of K-SiNPs. Hence, our fluorescent K-SiNPs can be used in the clinic to diagnose breast cellular carcinoma, since they can accurately measure the presence of invasive ductal carcinoma in serologic tests.


Assuntos
Neoplasias da Mama , Quempferóis , Teste de Materiais , Nanopartículas , Silício , beta-Galactosidase , Humanos , beta-Galactosidase/metabolismo , Silício/química , Células MCF-7 , Nanopartículas/química , Quempferóis/química , Quempferóis/farmacologia , Neoplasias da Mama/diagnóstico por imagem , Neoplasias da Mama/patologia , Tamanho da Partícula , Colorimetria , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Feminino , Estrutura Molecular
4.
ACS Appl Bio Mater ; 7(5): 3215-3226, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38695746

RESUMO

This study presents a tetra-substituted phthalonitrile derivative, namely, diethyl 2-(3,4-dicyano-2,5-bis(hexyloxy)-6-(4-(trifluoromethoxy)phenoxy)phenyl)malonate (a), cyclotetramerizing in the presence of some metal salts. The resultant hexadeca-substituted metal phthalocyanines [M= Co, Zn, InCl)] (b-d) were used for the modification of reduced graphene oxide for the first time. The effect of the phthalonitrile/metal phthalocyanines on biological features of reduced graphene oxide (rGO) was extensively examined by the investigation of antioxidant, antimicrobial, DNA cleavage, cell viability, and antibiofilm activities of nanobioagents (1-4). The results were compared with those of unmodified rGO (nanobioagent 5), as well. Modification of reduced graphene oxide with the synthesized compounds improved its antioxidant activity. The antioxidant activities of all the tested nanobioagents also enhanced as the concentration increased. The antibacterial activities of all the nanobioagents improved by applying the photodynamic therapeutic (PDT) method. All the phthalonitrile/phthalocyanine-based nanobioagents (especially phthalocyanine-based nanocomposites) exhibited DNA cleavage activities, and complete DNA fragmentation was observed for nanobioagents (1-4) at 200 mg/L. They can be used as potent antimicrobial and antimicrobial photodynamic therapy agents as well as Escherichia coli microbial cell inhibitors. As a result, the prepared nanocomposites can be considered promising candidates for biomedicine.


Assuntos
Antibacterianos , Materiais Biocompatíveis , Grafite , Indóis , Isoindóis , Teste de Materiais , Tamanho da Partícula , Grafite/química , Grafite/farmacologia , Indóis/química , Indóis/farmacologia , Antibacterianos/farmacologia , Antibacterianos/química , Antibacterianos/síntese química , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Testes de Sensibilidade Microbiana , Sobrevivência Celular/efeitos dos fármacos , Escherichia coli/efeitos dos fármacos , Estrutura Molecular , Biofilmes/efeitos dos fármacos , Humanos , Antioxidantes/farmacologia , Antioxidantes/química , Antioxidantes/síntese química , Óxidos/química , Óxidos/farmacologia
5.
ACS Appl Bio Mater ; 7(5): 3346-3357, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38695543

RESUMO

Septicemia, a severe bacterial infection, poses significant risks to human health. Early detection of septicemia by tracking specific biomarkers is crucial for a timely intervention. Herein, we developed a molecularly imprinted (MI) TiO2-Fe-CeO2 nanozyme array derived from Ce[Fe(CN)6] Prussian blue analogues (PBA), specifically targeting valine, leucine, and isoleucine, as potential indicators of septicemia. The synthesized nanozyme arrays were thoroughly characterized using various analytical techniques, including Fourier transform infrared spectroscopy, X-ray diffraction, field-emission scanning electron microscope, and energy-dispersive X-ray. The results confirmed their desirable physical and chemical properties, indicating their suitability for the oxidation of 3,3',5,5'-tetramethylbenzidine serving as a colorimetric probe in the presence of a persulfate oxidizing agent, further highlighting the potential of these arrays for sensitive and accurate detection applications. The MITiO2 shell selectively captures valine, leucine, and isoleucine, partially blocking the cavities for substrate access and thereby hindering the catalyzed TMB chromogenic reaction. The nanozyme array demonstrated excellent performance with linear detection ranges of 5 µM to 1 mM, 10-450 µM, and 10-450 µM for valine, leucine, and isoleucine, respectively. Notably, the corresponding limit of detection values were 0.69, 1.46, and 2.76 µM, respectively. The colorimetric assay exhibited outstanding selectivity, reproducibility, and performance in the detection of analytes in blood samples, including C-reactive protein at a concentration of 61 mg/L, procalcitonin at 870 ng/dL, and the presence of Pseudomonas aeruginosa bacteria. The utilization of Ce[Fe(CN)6]-derived MITiO2-Fe-CeO2 nanozyme arrays holds considerable potential in the field of septicemia detection. This approach offers a sensitive and specific method for early diagnosis and intervention, thereby contributing to improved patient outcomes.


Assuntos
Ferrocianetos , Sepse , Ferrocianetos/química , Sepse/diagnóstico , Sepse/microbiologia , Sepse/sangue , Humanos , Teste de Materiais , Tamanho da Partícula , Materiais Biocompatíveis/química , Materiais Biocompatíveis/síntese química , Impressão Molecular , Titânio/química , Cério/química , Colorimetria
6.
ACS Appl Bio Mater ; 7(5): 3506-3514, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38696441

RESUMO

Horseradish peroxidase (HRP)-mediated hydrogelation, caused by the cross-linking of phenolic groups in polymers in the presence of hydrogen peroxide (H2O2), is an effective route for bioink solidification in 3D bioprinting. Sugar beet pectin (SBP) naturally has cross-linkable phenols through the enzymatic reaction. Therefore, chemical modifications are not required, unlike the various polymers that have been used in the enzymatic cross-linking system. In this study, we report the application of SBP in extrusion-based bioprinting including HRP-mediated bioink solidification. In this system, H2O2 necessary for the solidification of inks is supplied in the gas phase. Cell-laden liver lobule-like constructs could be fabricated using bioinks consisting of 10 U/mL HRP, 4.0 and 6.0 w/v% SBP, and 6.0 × 106 cells/mL human hepatoblastoma (HepG2) cells exposed to air containing 16 ppm of H2O2 concurrently during printing and 10 min postprinting. The HepG2 cells enclosed in the printed constructs maintained their viability, metabolic activity, and hepatic functions from day 1 to day 7 of the culture, which indicates the cytocompatibility of this system. Taken together, this result demonstrates the potential of SBP and HRP cross-linking systems for 3D bioprinting, which can be applied in tissue engineering applications.


Assuntos
Beta vulgaris , Materiais Biocompatíveis , Bioimpressão , Peroxidase do Rábano Silvestre , Teste de Materiais , Pectinas , Impressão Tridimensional , Peroxidase do Rábano Silvestre/metabolismo , Peroxidase do Rábano Silvestre/química , Beta vulgaris/química , Humanos , Pectinas/química , Células Hep G2 , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Peróxido de Hidrogênio/química , Tamanho da Partícula , Sobrevivência Celular/efeitos dos fármacos , Reagentes de Ligações Cruzadas/química , Reagentes de Ligações Cruzadas/síntese química , Engenharia Tecidual
7.
ACS Appl Bio Mater ; 7(5): 3431-3440, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38697834

RESUMO

Light-induced release of cisplatin from Pt(IV) prodrugs represents a promising approach for precise control over the antiproliferative activity of Pt-based chemotherapeutic drugs. This method has the potential to overcome crucial drawbacks of conventional cisplatin therapy, such as high general toxicity toward healthy organs and tissues. Herein, we report two Pt(IV) prodrugs with BODIPY-based photoactive ligands Pt-1 and Pt-2, which were designed using carbamate and triazole linkers, respectively. Both prodrugs demonstrated the ability to release cisplatin under blue light irradiation without the requirement of an external reducing agent. Dicarboxylated Pt-2 prodrug turned out to be more stable in the dark and more sensitive to light than its monocarbamate Pt-1 counterpart; these observations were explained using DFT calculations. The investigation of the photoreduction mechanism of Pt-1 and Pt-2 prodrugs using DFT modeling and ΔG0 PET estimation suggests that the photoinduced electron transfer from the singlet excited state of the BODIPY axial ligand to the Pt(IV) center is the key step in the light-induced release of cisplatin from the complexes. Cytotoxicity studies demonstrated that both prodrugs were nontoxic in the dark and toxic to MCF-7 cells under low-dose irradiation with blue light, and the observed effect was solely due to the cisplatin release from the Pt(IV) prodrugs. Our research presents an elegant synthetic approach to light-activated Pt(IV) prodrugs and presents findings that may contribute to the future rational design of photoactivatable Pt(IV) prodrugs.


Assuntos
Antineoplásicos , Ensaios de Seleção de Medicamentos Antitumorais , Luz , Pró-Fármacos , Pró-Fármacos/química , Pró-Fármacos/farmacologia , Pró-Fármacos/síntese química , Humanos , Antineoplásicos/química , Antineoplásicos/farmacologia , Antineoplásicos/síntese química , Estrutura Molecular , Teste de Materiais , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Sobrevivência Celular/efeitos dos fármacos , Proliferação de Células/efeitos dos fármacos , Cisplatino/farmacologia , Cisplatino/química , Tamanho da Partícula , Compostos de Boro/química , Compostos de Boro/farmacologia , Compostos de Boro/síntese química , Processos Fotoquímicos , Teoria da Densidade Funcional
8.
ACS Appl Bio Mater ; 7(5): 2862-2871, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38699864

RESUMO

Mosquito-borne viruses are a major worldwide health problem associated with high morbidity and mortality rates and significant impacts on national healthcare budgets. The development of antiviral drugs for both the treatment and prophylaxis of these diseases is thus of considerable importance. To address the need for therapeutics with antiviral activity, a library of heparan sulfate mimetic polymers was screened against dengue virus (DENV), Yellow fever virus (YFV), Zika virus (ZIKV), and Ross River virus (RRV). The polymers were prepared by RAFT polymerization of various acidic monomers with a target MW of 20 kDa (average Mn ∼ 27 kDa by GPC). Among the polymers, poly(SS), a homopolymer of sodium styrenesulfonate, was identified as a broad spectrum antiviral with activity against all the tested viruses and particularly potent inhibition of YFV (IC50 = 310 pM). Our results further uncovered that poly(SS) exhibited a robust inhibition of ZIKV infection in both mosquito and human cell lines, which points out the potential functions of poly(SS) in preventing mosquito-borne viruses associated diseases by blocking viral transmission in their mosquito vectors and mitigating viral infection in patients.


Assuntos
Antivirais , Heparitina Sulfato , Polímeros , Antivirais/farmacologia , Antivirais/química , Antivirais/síntese química , Heparitina Sulfato/química , Heparitina Sulfato/farmacologia , Animais , Humanos , Polímeros/química , Polímeros/farmacologia , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Culicidae/efeitos dos fármacos , Culicidae/virologia , Testes de Sensibilidade Microbiana , Teste de Materiais , Tamanho da Partícula , Linhagem Celular , Estrutura Molecular , Chlorocebus aethiops , Materiais Biomiméticos/química , Materiais Biomiméticos/farmacologia , Zika virus/efeitos dos fármacos
9.
ACS Appl Bio Mater ; 7(5): 3337-3345, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38700956

RESUMO

A stimuli-responsive drug delivery nanocarrier with a core-shell structure combining photothermal therapy and chemotherapy for killing cancer cells was constructed in this study. The multifunctional nanocarrier ReS2@mSiO2-RhB entails an ReS2 hierarchical nanosphere coated with a fluorescent mesoporous silica shell. The three-dimensional hierarchical ReS2 nanostructure is capable of effectively absorbing near-infrared (NIR) light and converting it into heat. These ReS2 nanospheres were generated by a hydrothermal synthesis process leading to the self-assembly of few-layered ReS2 nanosheets. The mesoporous silica shell was further coated on the surface of the ReS2 nanospheres through a surfactant-templating sol-gel approach to provide accessible mesopores for drug uploading. A fluorescent dye (Rhodamine B) was covalently attached to silica precursors and incorporated during synthesis in the mesoporous silica walls toward conferring imaging capability to the nanocarrier. Doxorubicin (DOX), a known cancer drug, was used in a proof-of-concept study to assess the material's ability to function as a drug delivery carrier. While the silica pores are not capped, the drug molecule loading and release take advantage of the pH-governed electrostatic interactions between the drug and silica wall. The ReS2@mSiO2-RhB enabled a drug loading content as high as 19.83 mg/g doxorubicin. The ReS2@mSiO2-RhB-DOX nanocarrier's cumulative drug release rate at pH values that simulate physiological conditions showed significant pH responsiveness, reaching 59.8% at pH 6.8 and 98.5% and pH 5.5. The in vitro testing using HeLa cervical cancer cells proved that ReS2@mSiO2-RhB-DOX has a strong cancer eradication ability upon irradiation with an NIR laser owing to the combined drug delivery and photothermal effect. The results highlight the potential of ReS2@mSiO2-RhB nanoparticles for combined cancer therapy in the future.


Assuntos
Doxorrubicina , Liberação Controlada de Fármacos , Ensaios de Seleção de Medicamentos Antitumorais , Teste de Materiais , Nanopartículas , Tamanho da Partícula , Terapia Fototérmica , Rênio , Dióxido de Silício , Dióxido de Silício/química , Humanos , Doxorrubicina/farmacologia , Doxorrubicina/química , Concentração de Íons de Hidrogênio , Nanopartículas/química , Rênio/química , Rênio/farmacologia , Dissulfetos/química , Porosidade , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Sobrevivência Celular/efeitos dos fármacos , Antineoplásicos/química , Antineoplásicos/farmacologia , Portadores de Fármacos/química , Células HeLa
10.
ACS Appl Bio Mater ; 7(5): 3452-3459, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38723150

RESUMO

A two-photon nanoparticle probe was designed and developed based on the principle of intermolecular interaction of the aggregation-induced locally excited emission luminescence mechanism. The probe has the advantages of simple synthesis, convenient use, strong atomic economy, good biocompatibility, and photobleaching resistance. It can produce a specific and sensitive response to formaldehyde, help detect FA in normal cells and cancer cells, and is expected to become a specific detection probe for FA in vitro and in vivo.


Assuntos
Materiais Biocompatíveis , Formaldeído , Teste de Materiais , Nanopartículas , Tamanho da Partícula , Fótons , Formaldeído/química , Formaldeído/análise , Humanos , Nanopartículas/química , Materiais Biocompatíveis/química , Materiais Biocompatíveis/síntese química , Luminescência , Corantes Fluorescentes/química , Corantes Fluorescentes/síntese química , Estrutura Molecular
11.
Carbohydr Polym ; 337: 122143, 2024 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-38710552

RESUMO

Cyclodextrins (CDs) are essential in the pharmaceutical industry and have long been used as food and pharmaceutical additives. CD-based interlocked molecules, such as rotaxanes, polyrotaxanes, catenanes, and polycatenanes, have been synthesized and have attracted considerable attention in supramolecular chemistry. Among them, CD polyrotaxanes have been employed as slide-ring materials and biomaterials. CD polycatenanes are new materials; therefore, to date, no examples of applied research on CD polycatenanes have been reported. Consequently, we expect that applied research on CD polycatenanes will accelerate in the future. This review article summarizes the syntheses and structural analyses of CD polyrotaxanes and polycatenanes to facilitate their applications in the pharmaceutical industry. We believe that this review will promote further research on CD-based interlocked molecules.


Assuntos
Ciclodextrinas , Poloxâmero , Rotaxanos , Rotaxanos/química , Rotaxanos/síntese química , Ciclodextrinas/química , Ciclodextrinas/síntese química , Catenanos/química , Catenanos/síntese química , Materiais Biocompatíveis/química , Materiais Biocompatíveis/síntese química
12.
J Mater Chem B ; 12(19): 4574-4583, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38683108

RESUMO

Lipoic acid (LA) is a versatile antioxidant that has been used in the treatment of various oxidation-reduction diseases over the past 70 years. Owing to its large five-membered ring tension, the dynamic disulfide bond of LA is highly active, enabling the formation of poly(lipoic acid) (PLA) via ring-opening polymerization (ROP). Herein, we first summarize disulfide-mediated ROP polymerization strategies, providing basic routes for designing and preparing PLA-based materials. PLA, as a biologically derived, low toxic, and easily modified material, possesses dynamic disulfide bonds and universal non-covalent carboxyl groups. We also shed light on the biomedical applications of PLA-based materials based on their biological and structural features and further divide recent works into six categories: antibacterial, anti-inflammation, anticancer, adhesive, flexible electronics, and 3D-printed tissue scaffolds. Finally, the challenges and future prospects associated with the biomedical applications of PLA are discussed.


Assuntos
Materiais Biocompatíveis , Ácido Tióctico , Ácido Tióctico/química , Ácido Tióctico/farmacologia , Humanos , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Polímeros/química , Polímeros/farmacologia , Antineoplásicos/química , Antineoplásicos/farmacologia , Animais , Antibacterianos/química , Antibacterianos/farmacologia , Alicerces Teciduais/química , Anti-Inflamatórios/química , Anti-Inflamatórios/farmacologia , Polimerização , Antioxidantes/química , Antioxidantes/farmacologia
13.
ACS Appl Bio Mater ; 7(5): 3483-3495, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38685505

RESUMO

The two-dimensional (2D) WSe2 nanostructure was successfully synthesized via the hydrothermal method and subjected to comprehensive characterization using various spectroscopic techniques. X-ray diffraction (XRD) analysis confirmed the formation of nanosheets with a hexagonal crystal structure having a space symmetry of P63/mmc. Scanning electron microscopy (SEM) images showed irregular and nonuniform morphology. The size of the 2D nanosheets was determined using transmission electron microscopy (TEM) providing insights intotheir physical characteristics. The optical spectrum analysis yielded a discernible band gap value of 2.1 eV, as determined by the Tauc equation. Photoluminescence (PL) spectra display an emission at a wavelength of 610 nm, showing a broad emission associated with self-trapped excitons. Under excitation at λexc = 360 nm, PL emission spectra displayed a distinct peak at 610 nm, demonstrating the ability of the nanostructure to emit vivid red light. Photometric analysis underscored the potential of this nanostructure as a prominent red-light source for diverse display applications. The optimized photodetection performance of a device showcases a photoresponsivity of approximately 1.25 × 10-3 AW-1 and a detectivity of around 5.19 × 108 Jones at a wavelength of 390 nm. Additionally, the quantum efficiency is reported to be approximately 6.99 × 10-3 at a wavelength of 635 nm. These findings highlight the capability of the device for efficient photoconversion at specified wavelengths, indicating potential applications in sensing, imaging, and optical communication. The combination of structural, morphological, and optical characterizations highlights the suitability of 2D WSe2 nanostructure for practical optoelectronic applications, particularly in display technologies.


Assuntos
Teste de Materiais , Nanoestruturas , Tamanho da Partícula , Dispositivos Eletrônicos Vestíveis , Nanoestruturas/química , Materiais Biocompatíveis/química , Materiais Biocompatíveis/síntese química
14.
ACS Appl Bio Mater ; 7(5): 3033-3040, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38587908

RESUMO

Regenerative medicine based on cell therapy has emerged as a promising approach for the treatment of various medical conditions. However, the success of cell therapy heavily relies on the development of suitable injectable hydrogels that can encapsulate cells and provide a conducive environment for their survival, proliferation, and tissue regeneration. Herein, we address the medical need for cyto- and biocompatible injectable hydrogels by reporting on the synthesis of a hydrogel-forming thermosensitive copolymer. The copolymer was synthesized by grafting poly(N-isopropylacrylamide-co-carboxymethyl acrylate) (PNIPAM-COOH) onto chitosan through amide coupling. This chemical modification resulted in the formation of hydrogels that exhibit a sol-gel transition with an onset at approximately 27 °C, making them ideal for use in injectable applications. The hydrogels supported the survival and proliferation of cells for several days, which is critical for cell encapsulation. Furthermore, the study evaluates the addition of collagen/chitosan hybrid microspheres to support the adhesion of mesenchymal stem cells within the hydrogels. Altogether, these results demonstrate the potential of the PNIPAM-chitosan thermogel for cell encapsulation and its possible applications in regenerative medicine.


Assuntos
Resinas Acrílicas , Materiais Biocompatíveis , Quitosana , Hidrogéis , Teste de Materiais , Células-Tronco Mesenquimais , Microesferas , Quitosana/química , Resinas Acrílicas/química , Resinas Acrílicas/síntese química , Hidrogéis/química , Hidrogéis/síntese química , Hidrogéis/farmacologia , Células-Tronco Mesenquimais/citologia , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Tamanho da Partícula , Sobrevivência Celular/efeitos dos fármacos , Proliferação de Células/efeitos dos fármacos , Humanos
15.
ACS Appl Bio Mater ; 7(5): 3258-3270, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38593039

RESUMO

Reliable in vitro models closely resembling native tissue are urgently needed for disease modeling and drug screening applications. Recently, conductive biomaterials have received increasing attention in the development of in vitro models as they permit exogenous electrical signals to guide cells toward a desired cellular response. Interestingly, they have demonstrated that they promote cellular proliferation and adhesion even without external electrical stimulation. This paper describes the development of a conductive, fully synthetic hydrogel based on hybrids of the peptide-modified polyisocyanide (PIC-RGD) and the relatively conductive poly(aniline-co-N-(4-sulfophenyl)aniline) (PASA) and its suitability as the in vitro matrix. We demonstrate that incorporating PASA enhances the PIC-RGD hydrogel's electroactive nature without significantly altering the fibrous architecture and nonlinear mechanics of the PIC-RGD network. The biocompatibility of our model was assessed through phenotyping cultured human foreskin fibroblasts (HFF) and murine C2C12 myoblasts. Immunofluorescence analysis revealed that PIC-PASA hydrogels inhibit the fibrotic behavior of HFFs while promoting myogenesis in C2C12 cells without electrical stimulation. The composite PIC-PASA hydrogel can actively change the cell fate of different cell types, providing an attractive tool to improve skin and muscle repair.


Assuntos
Materiais Biocompatíveis , Hidrogéis , Teste de Materiais , Hidrogéis/química , Hidrogéis/farmacologia , Humanos , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Animais , Camundongos , Desenvolvimento Muscular/efeitos dos fármacos , Fibrose/tratamento farmacológico , Tamanho da Partícula , Fibroblastos/efeitos dos fármacos , Linhagem Celular , Estrutura Molecular , Proliferação de Células/efeitos dos fármacos , Condutividade Elétrica
16.
ACS Appl Bio Mater ; 7(5): 2794-2808, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38593040

RESUMO

In line with global goals to solve marine biofouling challenges, this study proposes an approach to developing a green synthesis inspired by natural resources for fouling-resistant behavior. A hybrid antifouling/foul release (HAF) coating based on poly(dimethylsiloxane) containing a green synthesized nanocomposite was developed as an environmentally friendly strategy. The nanocomposites based on graphene oxide (GO) and using marine sources, leaves, and stems of mangroves (Avicennia marina), brown algae (Polycladia myrica), and zinc oxide were compared. The effectiveness of this strategy was checked first in the laboratory and then in natural seawater. The performance stability of the coatings after immersion in natural seawater was also evaluated. With the lowest antifouling (17.95 ± 0.7%) and the highest defouling (51.2 ± 0.9%), the best fouling-resistant performance was for the coatings containing graphene oxide reduced with A. marina stem/zinc oxide (PrGZS) and graphene oxide reduced with A. marina leaves/zinc oxide with 50% multiwall carbon nanotubes (PrGZHC50), respectively. Therefore, the HAF coatings can be considered as developed and eco-friendly HAF coatings for the maritime industry.


Assuntos
Incrustação Biológica , Dimetilpolisiloxanos , Grafite , Interações Hidrofóbicas e Hidrofílicas , Teste de Materiais , Nanocompostos , Tamanho da Partícula , Propriedades de Superfície , Óxido de Zinco , Grafite/química , Dimetilpolisiloxanos/química , Nanocompostos/química , Óxido de Zinco/química , Incrustação Biológica/prevenção & controle , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química
17.
ACS Appl Bio Mater ; 7(5): 3014-3032, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38597359

RESUMO

Emission of greenhouse gases and infectious diseases caused by improper agro-waste disposal has gained significant attention in recent years. To overcome these hurdles, agro-waste can be valorized into valuable bioactive compounds that act as reducing or stabilizing agents in the synthesis of nanomaterials. Herein, we report a simple circular approach using Citrus reticulata Blanco (C. reticulata) waste (peel powder/aqueous extract) as green reducing and capping/stabilizing agents and Zn nitrate/acetate precursors to synthesize ZnO nanoparticles (NPs) with efficient antimicrobial and photocatalytic activities. The obtained NPs crystallized in a hexagonal wurtzite structure and differed clearly in their morphology. UV-vis analysis of the nanoparticles showed a characteristic broad absorption band between 330 and 414 nm belonging to ZnO NPs. Fourier transform infrared (FTIR) spectroscopy of ZnO NPs exhibited a Zn-O band close to 450 cm-1. The band gap values were in the range of 2.84-3.14 eV depending on the precursor and agent used. The crystallite size obtained from size-strain plots from measured XRD patterns was between 7 and 26 nm, with strain between 16 and 4%. The highly crystalline nature of obtained ZnO NPs was confirmed by clear ring diffraction patterns and d-spacing values of the observed lattice fringes. ZnNPeelMan_400 and ZnNExtrMan showed good stability, as the zeta potential was found to be around -20 mV, and reduced particle aggregation. Photoluminescence analysis revealed different defects belonging to oxygen vacancies (VO+ and VO+2) and zinc interstitial (Zni) sites. The presence of oxygen vacancies on the surface of ZnAcExtrMan_400 and ZnAcPeelMan_400 increased antimicrobial activity, specifically against Gram-negative bacteria Escherichia coli (E. coli) and Salmonella enteritidis (S. enteritidis). ZnNExtrMan with a minimal inhibitory concentration of 0.156 mg/mL was more effective against Gram-positive bacteria Staphylococcus aureus (S. aureus), revealing a high influence of particle size and shape on antimicrobial activity. In addition, the photocatalytic activity of the ZnO NPs was examined by assessing the degradation of acid green dye in an aqueous solution under UV light irradiation. ZnAcPeelMan_400 exhibited excellent photocatalytic activity (94%) within 90 min after irradiation compared to other obtained ZnO NPs.


Assuntos
Antibacterianos , Citrus , Teste de Materiais , Testes de Sensibilidade Microbiana , Tamanho da Partícula , Extratos Vegetais , Óxido de Zinco , Óxido de Zinco/química , Óxido de Zinco/farmacologia , Citrus/química , Antibacterianos/farmacologia , Antibacterianos/química , Antibacterianos/síntese química , Catálise , Extratos Vegetais/química , Extratos Vegetais/farmacologia , Escherichia coli/efeitos dos fármacos , Staphylococcus aureus/efeitos dos fármacos , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Processos Fotoquímicos , Nanopartículas Metálicas/química , Química Verde
18.
ACS Appl Bio Mater ; 7(5): 3227-3237, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38627897

RESUMO

2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofiber (TOCN) particles, an innovative biobased material derived from wood biomass, have garnered significant interest, particularly in the biomedical field, for their distinctive properties as biocompatible particle adsorbents. However, their microscopic size complicates their separation in liquid media, thereby impeding their application in various domains. In this study, superparamagnetic magnetite nanoparticles (NPs), specifically iron oxide Fe3O4 NPs with an average size of 15 nm, were used to enhance the collection efficiency of TOCN-Fe3O4 composite particles synthesized through spray drying. These composite particles exhibited a remarkable ζ-potential (approximately -50 mV), indicating their high stability in water, as well as impressive magnetization properties (up to 47 emu/g), and rapid magnetic responsiveness within 60 s in water (3 wt % Fe3O4 to TOCN, 1 T magnet). Furthermore, the influence of Fe3O4 NP concentrations on the measurement of the speed of magnetic separation was quantitatively discussed. Additionally, the binding affinity of the synthesized particles for proteins was assessed on a streptavidin-biotin binding system, offering crucial insights into their binding capabilities with specific proteins and underscoring their significant potential as functionalized biomedical materials.


Assuntos
Celulose , Nanopartículas Magnéticas de Óxido de Ferro , Teste de Materiais , Nanofibras , Tamanho da Partícula , Nanofibras/química , Celulose/química , Nanopartículas Magnéticas de Óxido de Ferro/química , Materiais Biocompatíveis/química , Materiais Biocompatíveis/síntese química , Nanopartículas de Magnetita/química
19.
ACS Appl Bio Mater ; 7(5): 3005-3013, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38629141

RESUMO

Freeze-based immobilization of deoxyribonucleic acid (DNA) oligonucleotides on gold nanoparticles (AuNPs) is highly efficient for single-stranded oligonucleotides but typically does not accommodate structures such as snap-cooled DNA hairpins (Sc-HPs) and snap-cooled molecular beacons (Sc-MBs) frequently used for biorecognition applications. Recognizing this limitation, we have developed a modified, freeze-based technique specifically designed to enable the adsorption of such hairpin oligonucleotides onto AuNP surfaces while ensuring that they retain their biosensing capabilities. Successful hairpin oligonucleotide conjugation of varying lengths to a wide range of AuNP diameters was corroborated by dynamic light scattering, ζ-potential, and UV-vis spectrophotometry. Moreover, we conducted a thorough evaluation of this modified method, confirming the retention of the sensing functions of Sc-HPs and Sc-MBs. This advancement not only offers a more efficient route for DNA hairpin conjugation but also elucidates the underlying biorecognition functions, with implications for broader applications in molecular diagnostics.


Assuntos
Técnicas Biossensoriais , DNA , Ouro , Nanopartículas Metálicas , Ouro/química , Nanopartículas Metálicas/química , DNA/química , Teste de Materiais , Tamanho da Partícula , Materiais Biocompatíveis/química , Materiais Biocompatíveis/síntese química
20.
ACS Appl Bio Mater ; 7(5): 3306-3315, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38634490

RESUMO

Photodynamic therapy (PDT) and ferroptosis show significant potential in tumor treatment. However, their therapeutic efficacy is often hindered by the oxygen-deficient tumor microenvironment and the challenges associated with efficient intracellular drug delivery into tumor cells. Toward this end, this work synthesized perfluorocarbon (PFC)-modified Pluronic F127 (PFC-F127), and then exploits it as a carrier for codelivery of photosensitizer Chlorin e6 (Ce6) and the ferroptosis promoter sorafenib (Sor), yielding an oxygen self-supplying nanoplatform denoted as Ce6-Sor@PFC-F127. The PFCs on the surface of the micelle play a crucial role in efficiently solubilizing and delivering oxygen as well as increasing the hydrophobicity of the micelle surface, giving rise to enhanced endocytosis by cancer cells. The incorporation of an oxygen-carrying moiety into the micelles enhances the therapeutic impact of PDT and ferroptosis, leading to amplified endocytosis and cytotoxicity of tumor cells. Hypotonic saline technology was developed to enhance the cargo encapsulation efficiency. Notably, in a murine tumor model, Ce6-Sor@PFC-F127 effectively inhibited tumor growth through the combined use of oxygen-enhanced PDT and ferroptosis. Taken together, this work underscores the promising potential of Ce6-Sor@PFC-F127 as a multifunctional therapeutic nanoplatform for the codelivery of multiple cargos such as oxygen, photosensitizers, and ferroptosis inducers.


Assuntos
Antineoplásicos , Clorofilídeos , Ensaios de Seleção de Medicamentos Antitumorais , Ferroptose , Fluorocarbonos , Micelas , Oxigênio , Fotoquimioterapia , Fármacos Fotossensibilizantes , Ferroptose/efeitos dos fármacos , Fluorocarbonos/química , Fluorocarbonos/farmacologia , Animais , Camundongos , Fármacos Fotossensibilizantes/química , Fármacos Fotossensibilizantes/farmacologia , Fármacos Fotossensibilizantes/síntese química , Humanos , Oxigênio/química , Antineoplásicos/química , Antineoplásicos/farmacologia , Antineoplásicos/síntese química , Teste de Materiais , Tamanho da Partícula , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/síntese química , Porfirinas/química , Porfirinas/farmacologia , Sobrevivência Celular/efeitos dos fármacos , Proliferação de Células/efeitos dos fármacos , Camundongos Endogâmicos BALB C , Sorafenibe/química , Sorafenibe/farmacologia , Sorafenibe/administração & dosagem , Poloxâmero/química , Linhagem Celular Tumoral , Neoplasias Experimentais/tratamento farmacológico , Neoplasias Experimentais/patologia , Neoplasias Experimentais/metabolismo , Estrutura Molecular
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