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1.
Angew Chem Int Ed Engl ; 63(8): e202317864, 2024 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-38189768

RESUMO

Nanoparticles can suppress asymmetric precursor support collapse during pyrolysis to create carbon molecular sieve (CMS) membranes. This advance allows elimination of standard sol-gel support stabilization steps. Here we report a simple but surprisingly important thermal soaking step at 400 °C in the pyrolysis process to obtain high performance CMS membranes. The composite CMS membranes show CO2 /CH4 (50 : 50) mixed gas feed with an attractive CO2 /CH4 selectivity of 134.2 and CO2 permeance of 71 GPU at 35 °C. Furthermore, a H2 /CH4 selectivity of 663 with H2 permeance of 240 GPU was achieved for promising green energy resource-H2 separation processes.

2.
Angew Chem Int Ed Engl ; 62(27): e202303915, 2023 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-37162173

RESUMO

Carbon molecular sieve (CMS) membranes are attractive candidates to meet requirements for challenging gas separations. The added ability to maintain such intrinsic properties in an asymmetric morphology with a structure that we term a "Pseudo Wheel+Hub & Spoke" asymmetric form offers new opportunities. For CMS membrane, specifically, the structure provides both selective layer support and low flow resistance even for high feed pressures and fluxes in CO2 removal from natural gas. This capability is unavailable to even rigid glassy polymers due to the much higher modulus of CMS materials. Combining precursor asymmetric hollow fiber formation and optimized pyrolysis creates a defect free CMS proof-of-concept membrane for this application. Facile formation of the sheath-core spun precursor with a 6FDA-DAM sheath and Matrimid® core also avoids the need to seal defects before or after the carbonization of the precursors. The composite CMS membrane shows CO2 /CH4 (50 : 50) mixed gas feed with an attractive CO2 /CH4 selectivity of 64.3 and CO2 permeance of 232 GPU at 35 °C. A key additional benefit of the approach is reduction in use of the more costly high performance 6FDA-DAM in a composite sheath-core CMS membrane with the "Pseudo Wheel+Hub & Spoke" structure.

3.
Nat Mater ; 22(1): 109-116, 2023 01.
Artigo em Inglês | MEDLINE | ID: mdl-36509871

RESUMO

Carbon molecular sieve (CMS) membranes with precise molecular discrimination ability and facile scalability are attractive next-generation membranes for large-scale, energy-efficient gas separations. Here, structurally engineered CMS membranes derived from a tailor-made cross-linkable copolyimide with kinked structure are reported. We demonstrate that combining two features, kinked backbones and cross-linkable backbones, to engineer polyimide precursors while controlling pyrolysis conditions allows the creation of CMS membranes with improved gas separation performance. Our results indicate that the CMS membranes provide a versatile platform for a broad spectrum of challenging gas separations. The gas transport properties of the resulting CMS membranes are interpreted in terms of a model reflecting both molecular sieving Langmuir domains and a disordered continuous phase, thereby providing insight into structure evolution from the cross-linkable polyimide precursor to a final CMS membrane. With this understanding of CMS membrane structure and separation performance, these systems are promising for environmentally friendly gas separations.


Assuntos
Carbono , Engenharia , Transporte Biológico , Pirólise
4.
Angew Chem Int Ed Engl ; 61(45): e202210831, 2022 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-36095046

RESUMO

Carbon molecular sieve (CMS) membranes offer the best available combination of scalable economical processability with excellent separation performance. Physical aging of CMS membranes causes pore structure changes over time that affect CMS membrane performance. To provide fundamental insights into the structure evolution in CMS membranes during physical aging, a combined dual-mode sorption and transport model is used in this study to characterize the diffusion coefficients of gas molecules in fresh and 7-day vacuum aged CMS membranes. The results show physical aging of CMS membrane is primarily "diffusion related" and such aging behavior simultaneously causes ultramicropore changes in the continuous phase and Langmuir phase of CMS membrane. The new insights offered in this study suggest strategies to control the physical aging of CMS membranes and even use it as a valuable tool to tune the separation performance of CMS membranes for demanding gas separations.

5.
Angew Chem Int Ed Engl ; 60(41): 22322-22331, 2021 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-34347936

RESUMO

Carbon molecular sieve (CMS) membranes have impressive separation properties; however, both chemical and morphology structures need to be understood better. Here we characterize CMS with the simplest polyimide (PI) PMDA/pPDA (PMDA=pyromellitic dianhydride, pPDA=p-phenylenediamine), using FTIR, solid-state 15 N-NMR and 13 C-NMR, XPS, XRD, and Raman spectra to study chemical structure. We also compare gas separation properties for this CMS to a CMS derived from a more conventional PI precursor. The detailed characterization shows the presence of aromatic pyridinic, pyrrolic rings as well as graphitic, pyridonic components and a few other groups in both CMS types derived from the very different precursors. The CMS morphologies, while related to precursor and pyrolysis temperature details, show similarities consistent with a physical picture comprising distributed molecular sieving plate-like structures. These results assist in understanding diverse CMS membrane separation performance.

6.
ACS Appl Mater Interfaces ; 13(25): 29726-29736, 2021 Jun 30.
Artigo em Inglês | MEDLINE | ID: mdl-34137583

RESUMO

The low-cost and high-capacity micron silicon is identified as the suitable anode material for high-performance lithium-ion batteries (LIBs). However, the particle fracture and severe capacity fading during electrochemical cycling greatly impede the practical application of LIBs. Herein, we first proposed an in situ reduction and template assembly strategy to attain a weave cage-like carbon nanostructure, composed of short carbon nanotubes and small graphene flakes, as a flexible nanotemplate that closely wrapped micron-sized mesoporous silicon (PSi) to form a robust composite construction. The in situ formed weave cage-like carbon nanostructure can remarkably improve the electrochemical property and structural stability of micron-sized PSi during deep galvanostatic cycling and high electric current density owing to multiple attractive advantages. As a result, the rechargeable LIB applying this anode material exhibits improved initial Coulombic efficiency (ICE), excellent rate performance, and cyclic stability in the existing micron-sized PSi/nanocarbon system. Moreover, this anode reached an approximation of 100% ICE after only three cycles and maintains this level in subsequent cycles. This design of flexible nanotemplated platform wrapped micron-sized PSi anode provides a steerable nanoengineering strategy toward conquering the challenge of long-term reliable LIB application.

7.
ACS Omega ; 5(42): 27368-27373, 2020 Oct 27.
Artigo em Inglês | MEDLINE | ID: mdl-33134699

RESUMO

Nanostructured hollow silicon has attracted tremendous attention as high-performance anode materials in Li-ion battery applications. However, the large-scale production of pure hollowed silicon with long cycling stability is still a great challenge. Here, we report an improved low-temperature molten salt strategy to synthesize nanosized hollowed silicon with a stable structure on a large scale. As an anode material for rechargeable lithium-ion batteries, it exhibits a high capacity, excellent long cycling, and steady rate performance at different current densities. Especially, a high reversible capacity of 2028.6 mA h g-1 at 0.5 A g-1 after 150 cycles, 994.3 mA h g-1 at 3 A g-1 after 500 cycles, and 538.8 mAh g-1 at 5 A g-1 after 1200 cycles could be obtained. This kind of nanosized hollowed silicon can be applied as a basic anode material in silicon-based composites for long-term stable Li-ion battery applications.

8.
Angew Chem Int Ed Engl ; 59(35): 14877-14883, 2020 08 24.
Artigo em Inglês | MEDLINE | ID: mdl-32365260

RESUMO

Glassy polyimide membranes are attractive for industrial applications in sour natural gas purification. Unfortunately, the lack of fundamental understanding of relationships between polyimide chemical structures and their gas transport properties in the presence of H2 S constrains the design and engineering of advanced membranes for such challenging applications. Herein, 6FDA-based polyimide membranes with engineered structures were synthesized to tune their CO2 /CH4 and H2 S/CH4 separation performances and plasticization properties. Under ternary mixed sour gas feeds, controlling polymer chain packing and plasticization tendency of such polyimide membranes via tuning the chemical structures were found to offer better combined H2 S and CO2 removal efficiency compared to conventional polymers. Fundamental insights into structure-property relationships of 6FDA-based polyimide membranes observed in this study offer guidance for next generation membranes for sour natural gas separation.

9.
ACS Omega ; 4(19): 18195-18202, 2019 Nov 05.
Artigo em Inglês | MEDLINE | ID: mdl-31720520

RESUMO

Considering the sharp increase in energy demand, Si-based composites have shown promise as high-performance anodes for lithium-ion batteries during the last few years. However, a significant volume change of Si during repetitive cycles may cause technical and security problems that limit the particular application. Here, an optimized reduced graphene oxide/silicon (RGO/Si) composite with excellent stability has been fabricated via a facile templated self-assembly strategy. The active silicon nanoparticles were uniformly supported by graphene that can further form a three-dimensional network to buffer the volume change of Si and produce a stable solid-electrolyte interphase film due to the increased specific surface area and enhanced intermolecular interaction, resulting in an increase of electrical conductivity and structural stability. As the anode electrode material of lithium-ion batteries, the optimized 10RGO/Si-600 composite showed a reversible high capacity of 2317 mA h/g with an initial efficiency of 93.2% and a quite high capacity retention of 85% after 100 cycles at 0.1 A/g rate. Especially, it still displayed a specific capacity of 728 mA h/g after 100 cycles at a reasonably high current density of 2 A/g. This study has proposed the optimized method for developing advanced graphene/Si nanocomposites for enhanced cycling stability lithium-ion batteries.

10.
Environ Sci Technol ; 52(17): 9684-9693, 2018 09 04.
Artigo em Inglês | MEDLINE | ID: mdl-30074383

RESUMO

Forward osmosis (FO) has gained increasing attention in desalination, wastewater treatment, and power generation. However, biofouling remains a major obstacle for the sustainable development of the FO process. Both passive and active strategies have been developed to mitigate membrane biofouling. A comprehensive understanding of different strategies and mechanisms has fundamental significance for the antifouling membrane development. In this study, thin-film composite (TFC) FO membranes were modified with polydopamine (PDA) coating as a passive antibacterial moiety and silver nanoparticles (Ag NPs) as an active antibacterial moiety. Their anti-biofouling performances were investigated both in static and dynamic conditions. In static exposure, the PDA-coated membranes exhibited great passive anti-adhesive property, and the Ag-NP-generated membranes presented both of excellent passive anti-adhesive properties and active antibacterial performance. While in dynamic cross-flow running conditions, Ag NPs effectively mitigated the membrane water flux decline due to their inhibition of biofilm growth, the PDA coating failed because of its inability to inactivate the attached bacteria growth. Moreover, Ag NPs were stable and active on membrane surfaces after 24 h of cross-flow operation. These findings provide new insights into the performances and mechanisms of passive and active moieties in the FO process.


Assuntos
Incrustação Biológica , Nanopartículas Metálicas , Purificação da Água , Membranas Artificiais , Osmose , Prata
11.
ACS Appl Mater Interfaces ; 9(46): 40987-40997, 2017 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-29111650

RESUMO

We developed a simple and facile approach to covalently immobilize Ag nanoparticles (NPs) onto polyamide surfaces of thin film composite membranes through layer-by-layer interfacial polymerization (LBL-IP) for biofouling mitigation. Stable and uniform bovine serum albumin (BSA) capped Ag NPs with an average diameter of around 20 nm were synthesized using BSA as a template under the assistance of sonication, and Ag NPs incorporated thin film composite (TFC) polyamide membrane was then fabricated by LBL-IP on a nanoporous polysulfone (PSf) substrate upon sequential coating with m-phenylenediamine (MPD) aqueous solution, trimesoyl chloride (TMC)-hexane solution, and finally BSA-capped Ag NPs aqueous solution. The influence of Ag NPs incorporation was investigated on the surface physicochemical properties, water permeability, and salt rejection of TFC polyamide membrane. Our findings show that Ag NPs functionalized membrane exhibited excellent antibacterial properties without sacrificing their permeability and rejection, and Ag NPs incorporation affected very little surface roughness and charge of polyamide layer. Moreover, the incorporated Ag NPs presented a low release rate and excellent stability on polyamide surface in cross-flow conditions. Given the simplicity and versatility of this approach, our study provides a practicable avenue for direct incorporation of various surface-tailored nanomaterials on the polyamide surface to develop high-performance TFC membranes with fouling-resistant properties on a large scale.


Assuntos
Nanopartículas Metálicas , Antibacterianos , Membranas Artificiais , Nylons , Polimerização , Prata
12.
Oncol Rep ; 38(5): 2919-2926, 2017 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-28901480

RESUMO

The aim of this study was to look for a new medicine in diagnosing and treating of glioblastoma. Radioiodine-labeled anti-epidermal growth factor receptor (EGFR) binding nanoparticles were constructed. In vitro cell-binding assays were confirmed by confocal microscopy and flow cytometry. Cell cytotoxicity assays were evaluated by MTT assay; radionuclide uptake assays were performed by γ-counter. Radioiodine-imaging studies were conducted using a xenograft nude mouse model in vivo. The results showed that EGFR significantly enhanced the uptake and accumulation of BSA-PCL in the experimental model of xenografts in nude mice, suggesting improved specific nanoparticle-based delivery. In conclusion, the data showed 131I-EGFR-BSA-PCL leading radioiodine therapy for U251 and U87 cells had a good effect in vitro and in vivo. Thus, 131I-EGFR-BSA-PCL may provide a new method for glioblastoma treatment.


Assuntos
Neoplasias Encefálicas/diagnóstico por imagem , Neoplasias Encefálicas/tratamento farmacológico , Cetuximab/administração & dosagem , Glioblastoma/diagnóstico por imagem , Glioblastoma/tratamento farmacológico , Radioisótopos do Iodo/administração & dosagem , Compostos Radiofarmacêuticos/administração & dosagem , Animais , Neoplasias Encefálicas/metabolismo , Bovinos , Linhagem Celular Tumoral , Sobrevivência Celular/efeitos dos fármacos , Cetuximab/química , Cetuximab/farmacologia , Receptores ErbB/metabolismo , Glioblastoma/metabolismo , Humanos , Radioisótopos do Iodo/química , Camundongos , Nanopartículas/administração & dosagem , Nanopartículas/química , Transplante de Neoplasias , Poliésteres/administração & dosagem , Poliésteres/química , Compostos Radiofarmacêuticos/química , Soroalbumina Bovina/administração & dosagem , Soroalbumina Bovina/química , Tomografia Computadorizada de Emissão de Fóton Único/métodos , Ensaios Antitumorais Modelo de Xenoenxerto
13.
ACS Appl Mater Interfaces ; 8(48): 32688-32698, 2016 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-27934134

RESUMO

Combined cancer therapy possesses many advantages including improved tumoricidal efficacy, reduced side effects, and retarded drug resistance. Herein, a protein-polymer bioconjugate-coated multifunctional upconversion nanosystem, consisting of upconversion nanoparticles (UCNs) core, tailored amphiphilic protein-polymer bioconjugate shell, and photosensitizer zinc phthalocyanine (ZnPc) and antitumor drug doxorubicin coloaded inside, was elaborately developed for combined photodynamic therapy (PDT) and chemotherapy. In this system, UCNs core could convert deep penetrating near-infrared light to visible light for simultaneous cell fluorescence imaging and photodynamic therapy by activating ZnPc to generate cytotoxic ROS, while the protective shell of bovine serum albumin-poly(ε-caprolactone) (BSA-PCL) offered excellent water solubility, good stability, and low cytotoxicity. The ROS production test showed that this nanosystem could successfully generate singlet oxygen under NIR irradiation. A cellular uptake study demonstrated that intense fluorescence emission of the UCNs could be observed in HeLa cells, indicating their outstanding real-time imaging capability. More importantly, compared with single PDT or chemotherapy systems, the constructed combined therapy UCNs system demonstrated significantly enhanced tumor cell killing efficiency. On the basis of our findings, this multifunctional UCNs nanosystem could be a promising versatile theranostic nanoplatform for image-guided combined cancer therapy.


Assuntos
Doxorrubicina/administração & dosagem , Indóis/administração & dosagem , Nanopartículas/administração & dosagem , Nanopartículas/química , Compostos Organometálicos/administração & dosagem , Fotoquimioterapia/métodos , Neoplasias do Colo do Útero/diagnóstico por imagem , Neoplasias do Colo do Útero/tratamento farmacológico , Antibióticos Antineoplásicos/administração & dosagem , Antibióticos Antineoplásicos/química , Antibióticos Antineoplásicos/farmacocinética , Doxorrubicina/química , Doxorrubicina/farmacocinética , Portadores de Fármacos/administração & dosagem , Portadores de Fármacos/química , Portadores de Fármacos/farmacocinética , Sistemas de Liberação de Medicamentos/métodos , Feminino , Células HeLa , Humanos , Indóis/química , Indóis/farmacocinética , Isoindóis , Compostos Organometálicos/química , Compostos Organometálicos/farmacocinética , Fármacos Fotossensibilizantes/administração & dosagem , Fármacos Fotossensibilizantes/química , Fármacos Fotossensibilizantes/farmacocinética , Poliésteres/administração & dosagem , Poliésteres/química , Poliésteres/farmacocinética , Espécies Reativas de Oxigênio/metabolismo , Soroalbumina Bovina/administração & dosagem , Soroalbumina Bovina/química , Soroalbumina Bovina/farmacocinética , Neoplasias do Colo do Útero/metabolismo , Compostos de Zinco
14.
Chem Commun (Camb) ; 52(82): 12245-12248, 2016 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-27711271

RESUMO

A one-pot method was developed for the chelation of copper ions onto the surface of filtration membrane to provide antibacterial properties. This simple, universal and cost-effective dopamine-Cu2+ approach provides a method of mitigating the long-term biofouling of surfaces.


Assuntos
Antibacterianos/farmacologia , Incrustação Biológica/prevenção & controle , Cobre/química , Dopamina/química , Membranas Artificiais , Staphylococcus aureus/efeitos dos fármacos , Antibacterianos/química , Filtração , Propriedades de Superfície
15.
ACS Appl Mater Interfaces ; 8(33): 21666-73, 2016 Aug 24.
Artigo em Inglês | MEDLINE | ID: mdl-27467542

RESUMO

Microbial attachment and biofilm formation on filtration membrane can greatly compromise its flux and separation efficiency. Here, a simple and facile approach has been developed to in situ generate silver nanoparticles (Ag NPs) on the thin film composite forward osmosis (TFC FO) membrane for sustainable antibiofouling performances. Mussel-inspired dopamine chemistry was applied to grow polydopamine coating on both surfaces of FO membranes, followed by the generation of Ag NPs upon a simple dip coating in silver nitrate aqueous solution. Furthermore, the Ag NPs deposited membranes had a long-term silver release profile with rechargability for multiple times upon their depletion, and exhibited strong sustainable bactericidal efficacy against Gram-negative bacteria and Gram-positive bacteria. The Ag NPs had a controllable effect on the membrane performances including the water flux and reverse salt flux in the FO test mode. Our practicable antibacterial strategy may apply to other types of filtration membranes with diverse material surfaces and may pave a new way to achieve the sustainable membrane antibiofouling performance on a large scale.

16.
Adv Healthc Mater ; 5(17): 2214-26, 2016 09.
Artigo em Inglês | MEDLINE | ID: mdl-27253762

RESUMO

Considering the critical role of mitochondria in the life and death of cells, non-invasive long-term tracking of mitochondria has attracted considerable interest. However, a high-performance mitochondria-specific labeling probe with high photostability is still lacking. Herein a highly photostable hyperbranched polyglycerol (hPG)-based near-infrared (NIR) quantum dots (QDs) nanoplatform is reported for mitochondria-specific cell imaging. Comprising NIR Zn-Cu-In-S/ZnS QDs as extremely photostable fluorescent labels and alkyl chain (C12 )/triphenylphosphonium (TPP)-functionalized hPG derivatives as protective shell, the tailored QDs@hPG-C12 /TPP nanoprobe with a hydrodynamic diameter of about 65 nm exhibits NIR fluorescence, excellent biocompatibility, good stability, and mitochondria-targeted ability. Cell uptake experiments demonstrate that QDs@hPG-C12 /TPP displays a significantly enhanced uptake in HeLa cells compared to nontargeted QDs@hPG-C12 . Further co-localization study indicates that the probe selectively targets mitochondria. Importantly, compared with commercial deep-red mitochondria dyes, QDs@hPG-C12 /TPP possesses superior photostability under continuous laser irradiation, indicating great potential for long-term mitochondria labeling and tracking. Moreover, drug-loaded QDs@hPG-C12 /TPP display an enhanced tumor cell killing efficacy compared to nontargeted drugs. This work could open the door to the construction of organelle-targeted multifunctional nanoplatforms for precise diagnosis and high-efficient tumor therapy.


Assuntos
Sistemas de Liberação de Medicamentos/métodos , Glicerol , Mitocôndrias/metabolismo , Polímeros , Pontos Quânticos/química , Glicerol/química , Glicerol/farmacologia , Células HeLa , Humanos , Microscopia de Fluorescência/métodos , Polímeros/química , Polímeros/farmacologia
17.
World J Gastroenterol ; 22(14): 3758-68, 2016 Apr 14.
Artigo em Inglês | MEDLINE | ID: mdl-27076760

RESUMO

AIM: To investigate the biological effects of internal irradiation, and the therapeutic effectiveness was assessed of (131)I-labeled anti-epidermal growth factor receptor (EGFR) liposomes, derived from cetuximab, when used as a tumor-targeting carrier in a colorectal cancer mouse model. METHODS: We described the liposomes and characterized their EGFR-targeted binding and cellular uptake in EGFR-overexpressing LS180 colorectal cancer cells. After intra-tumor injections of 74 MBq (740 MBq/mL) (131)I-antiEGFR-BSA-PCL, we investigated the biological effects of internal irradiation and the therapeutic efficacy of (131)I-antiEGFR-BSA-PCL on colorectal cancer in a male BALB/c mouse model. Tumor size, body weight, histopathology, and SPECT imaging were monitored for 33 d post-therapy. RESULTS: The rapid radioiodine uptake of (131)I-antiEGFR-BSA-PCL and (131)I-BSA-PCL reached maximum levels at 4 h after incubation, and the (131)I uptake of (131)I-antiEGFR-BSA-PCL was higher than that of (131)I-BSA-PCL in vitro. The (131)I tissue distribution assay revealed that (131)I-antiEGFR-BSA-PCL was markedly taken up by the tumor. Furthermore, a tissue distribution assay revealed that (131)I-antiEGFR-BSA-PCL was markedly taken up by the tumor and reached its maximal uptake value of 21.0 ± 1.01 %ID/g (%ID/g is the percentage injected dose per gram of tissue) at 72 h following therapy; the drug concentration in the tumor was higher than that in the liver, heart, colon, or spleen. Tumor size measurements showed that tumor development was significantly inhibited by treatments with (131)I-antiEGFR-BSA-PCL and (131)I-BSA-PCL. The volume of tumor increased, and treatment rate with (131)I-antiEGFR-BSA-PCL was 124% ± 7%, lower than that with (131)I-BSA-PCL (127% ± 9%), (131)I (143% ± 7%), and normal saline (146% ± 10%). The percentage losses in original body weights were 39% ± 3%, 41% ± 4%, 49% ± 5%, and 55% ± 13%, respectively. The best survival and cure rates were obtained in the group treated with (131)I-antiEGFR-BSA-PCL. The animals injected with (131)I-antiEGFR-BSA-PCL and (131)I-BSA-PCL showed more uniform focused liposome distribution within the tumor area. CONCLUSION: This study demonstrated the potential beneficial application of (131)I-antiEGFR-BSA-PCL for treating colorectal cancer. (131)I-antiEGFR-BSA-PCL suppressed the development of xenografted colorectal cancer in nude mice, thereby providing a novel candidate for receptor-mediated targeted radiotherapy.


Assuntos
Cetuximab/farmacologia , Neoplasias Colorretais/radioterapia , Receptores ErbB/antagonistas & inibidores , Radioisótopos do Iodo/farmacologia , Poliésteres/farmacologia , Compostos Radiofarmacêuticos/farmacologia , Soroalbumina Bovina/farmacologia , Animais , Linhagem Celular Tumoral , Neoplasias Colorretais/imunologia , Neoplasias Colorretais/metabolismo , Neoplasias Colorretais/patologia , Receptores ErbB/imunologia , Receptores ErbB/metabolismo , Feminino , Humanos , Radioisótopos do Iodo/farmacocinética , Lipossomos , Camundongos Endogâmicos BALB C , Camundongos Nus , Microscopia Confocal , Terapia de Alvo Molecular , Nanopartículas , Poliésteres/farmacocinética , Compostos Radiofarmacêuticos/farmacocinética , Soroalbumina Bovina/farmacocinética , Nanomedicina Teranóstica , Distribuição Tecidual , Tomografia Computadorizada de Emissão de Fóton Único , Carga Tumoral/efeitos dos fármacos , Ensaios Antitumorais Modelo de Xenoenxerto
18.
J Cancer Res Clin Oncol ; 142(3): 619-32, 2016 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-26573511

RESUMO

INTRODUCTION: Anti-epidermal growth factor receptor (EGFR)-targeted nanoparticles can be used to deliver a therapeutic and imaging agent to EGFR-overexpressing tumor cells. (131)I-labeled anti-EGFR nanoparticles derived from cetuximab were used as a tumor-targeting vehicle in radionuclide therapy. METHODS: This paper describes the construction of the anti-EGFR nanoparticle EGFR-BSA-PCL. This nanoparticle was characterized for EGFR-targeted binding and cellular uptake in EGFR-overexpressing cancer cells by using flow cytometry and confocal microscopy. Anti-EGFR and non-targeted nanoparticles were labeled with (131)I using the chloramine-T method. Analyses of cytotoxicity and targeted cell killing with (131)I were performed using the MTT assay. The time-dependent cellular uptake of (131)I-labeled anti-EGFR nanoparticles proved the slow-release effects of nanoparticles. A radioiodine therapy study was also performed in mice. RESULTS: The EGFR-targeted nanoparticle EGFR-BSA-PCL and the non-targeted nanoparticle BSA-PCL were constructed; the effective diameters were approximately 100 nm. The results from flow cytometry and confocal microscopy revealed significant uptake of EGFR-BSA-PCL in EGFR-overexpressing tumor cells. Compared with EGFR-BSA-PCL, BSA-PCL could also bind to cells, but tumor cell retention was minimal and weak. In MTT assays, the EGFR-targeted radioactive nanoparticle (131)I-EGFR-BSA-PCL showed greater cytotoxicity and targeted cell killing than the non-targeted nanoparticle (131)I-BSA-PCL. The radioiodine uptake of both (131)I-labeled nanoparticles, (131)I-EGFR-BSA-PCL and (131)I-BSA-PCL, was rapid and reached maximal levels 4 h after incubation, but the (131)I uptake of (131)I-EGFR-BSA-PCL was higher than that of (131)I-BSA-PCL. On day 15, the average tumor volumes of the (131)I-EGFR-BSA-PCL and (131)I-BSA-PCL groups showed a slow growth relationship compared with that of the control group. CONCLUSION: The EGFR-targeted nanoparticle EGFR-BSA-PCL demonstrated superior cellular binding and uptake compared with those of the control BSA-PCL. The EGFR-targeted radioactive nanoparticle (131)I-EGFR-BSA-PCL exhibited favorable intracellular retention of (131)I. Radionuclide therapy using (131)I-EGFR-BSA-PCL, which showed excellent targeted cell killing, suppressed cancer cell growth caused by EGFR overexpression.


Assuntos
Anticorpos Monoclonais Humanizados/farmacologia , Receptores ErbB/genética , Radioisótopos do Iodo/farmacologia , Neoplasias/genética , Neoplasias/radioterapia , Animais , Anticorpos Monoclonais Humanizados/administração & dosagem , Linhagem Celular Tumoral , Cetuximab/administração & dosagem , Cetuximab/farmacologia , Sistemas de Liberação de Medicamentos , Receptores ErbB/antagonistas & inibidores , Receptores ErbB/imunologia , Feminino , Regulação Neoplásica da Expressão Gênica , Humanos , Radioisótopos do Iodo/administração & dosagem , Camundongos , Camundongos Endogâmicos BALB C , Camundongos Nus , Terapia de Alvo Molecular/métodos , Nanopartículas/administração & dosagem , Neoplasias/patologia , Ensaios Antitumorais Modelo de Xenoenxerto
19.
ACS Appl Mater Interfaces ; 7(34): 18997-9005, 2015 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-26262596

RESUMO

A simple, straightforward, and reproducible strategy for the construction of a near-infrared (NIR) fluorescence nanoprobe was developed by coating CuInS2/ZnS quantum dots (CIS/ZnS QDs) with a novel amphiphilic bioconjugate. The amphiphilic bioconjugate with a tailor-designed structure of bovine serum albumin (BSA) as the hydrophilic segment and poly(ε-caprolactone) (PCL) as the hydrophobic part was fabricated by chemical coupling the hydrophobic polymer chain to BSA via the maleimide-sulfhydryl reaction. By incorporating CIS/ZnS QDs into the hydrophobic cores of the self-assembly of BSA-PCL conjugate, the constructed NIR fluorescence nanoprobe exhibited excellent fluorescent properties over a wide pH range (pH 3-10) and a good colloidal stability in PBS buffer (pH = 7.4) with or without 10% fetal bovine serum. The presence of the outer BSA shell effectively reduced the nonspecific cellular binding and imparted high biocompatibility and low-toxicity to the probe. Moreover, the NIR fluorescence nanoprobe could be functionalized by conjugating cyclic Arg-Gly-Asp (cRGD) peptide, and the decorated nanoprobe was shown to be highly selective for targeted integrin αvß3-overexpressed tumor cell imaging. The feasibility of the constructed NIR fluorescence probe in vivo application was further investigated and the results demonstrated its great potential for in vivo imaging. This developed protocol for phase transfer of the CIS/ZnS QDs was universal and applicable to other nanoparticles stabilized with hydrophobic ligands.


Assuntos
Imagem Molecular/métodos , Nanopartículas/química , Nanotecnologia/métodos , Poliésteres/química , Soroalbumina Bovina/metabolismo , Espectroscopia de Luz Próxima ao Infravermelho , Tensoativos/química , Animais , Bovinos , Morte Celular , Sobrevivência Celular , Feminino , Células HeLa , Humanos , Camundongos Nus , Pontos Quânticos/química , Pontos Quânticos/ultraestrutura , Espectrometria de Fluorescência , Espectrometria de Massas por Ionização e Dessorção a Laser Assistida por Matriz , Sulfetos/química , Compostos de Zinco/química
20.
ACS Appl Mater Interfaces ; 7(14): 7566-75, 2015 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-25799279

RESUMO

Inspired by the specificity of acid tumor microenvironment, we constructed a flexible charge-reversible near-infrared (NIR) fluorescence nanoprobe in response to tumor extracellular pH (pHe) for effective tumor-specific imaging. The nanoprobe consists of an NIR-emitted CuInS2/ZnS quantum dot (CIS/ZS QDs) core and a tailored lauric acid and 2,3-dimethylmaleic anhydride modified ε-polylysine (ε-PL-g-LA/DMA) shell, which provides not only a dense protective layer for the QDs but also the ability of pHe-induced positive charge-mediated endocytosis into tumor cells. The results showed that the QDs@ε-PL-g-LA/DMA nanoprobe with a uniform size of 40 nm had high chemical stability at pH 7.4 and excellent optical properties. Especially, it swiftly reversed its surface charge to positive in 20 min when exposed to pHe due to the cleavage of the ß-carboxyl amide bond of ε-PL-g-LA/DMA. Moreover, the cell uptake of the pHe-sensitive QDs nanoprobe exposed at pH 6.8 into HeLa cells is much more significant than that at pH 7.4, which further verified the availability of the electrostatic adsorptive endocytosis facilitated targeting ability. The pHe-induced targeting imparted the QDs nanoprobe a broad targeting ability in a variety of solid tumors. Furthermore, as an effective alternative mechanism for tumor targeting, responsive charge reversion is also universally applicable to other cancer theranostics agent.


Assuntos
Microscopia de Fluorescência/métodos , Técnicas de Sonda Molecular , Nanocápsulas/química , Pontos Quânticos , Espectroscopia de Luz Próxima ao Infravermelho/métodos , Frações Subcelulares/ultraestrutura , Células HeLa , Humanos , Concentração de Íons de Hidrogênio , Sondas Moleculares/química , Nanocápsulas/ultraestrutura , Eletricidade Estática
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