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1.
J Am Chem Soc ; 142(2): 978-986, 2020 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-31841620

RESUMO

Sulfur utilization is a global concern because of its abundant nature sources and the safety or environmental problems caused by its burning or oxidation during storage, while sulfur-containing polymers are popular materials in virtue of their fascinating properties such as metal coordination ability, high refractive indices, and semiconducting property. The synthesis of sulfur-containing polymers is challenging, especially directly from elemental sulfur. Herein, catalyst-free and scalable multicomponent polymerizations (MCPs) of all commercially available elemental sulfur, dicarboxylic acids, and diamines were reported to facilely construct 12 polythioamides with diverse and well-defined structures, high molecular weights (Mw's up to 86 200 g/mol), and excellent yields (up to 99%) from elemental sulfur. Besides commonly used aliphatic diamines, aromatic diamine monomers are also applicable to these multicomponent polymerizations, affording polythioamides with unique rigid structures and improved functionality as compared to those of the previously reported polythioamides. These polythioamides can be applied in gold recovery, which could extract a trace amount of Au3+ from practical acidic leaching solution of discarded electronic waste selectively, rapidly (1 min), sensitively (10 ppb), and efficiently (>99.99%) with high extraction capacity up to 0.60 g· Au3+/g to directly afford high-purity elemental gold after pyrolysis. The MCPs could make use of both abundantly existing sulfur waste and trace amounts of precious gold residue in electronic wastes, demonstrating their great potential in resource utilization.

2.
Mater Sci Eng C Mater Biol Appl ; 96: 684-692, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30606582

RESUMO

The immobilization of photo-catalyst can effectively avoid the difficulty in recovery of the nano-catalysts after photo-degradation. In this work, PVDF/GO/ZnO composite membranes with photocatalytic performance for organic dyes were prepared by using zinc oxide (ZnO) as photo-catalyst, graphene (GO) as dispersant and poly (vinylidene fluoride) (PVDF) membrane as carrier. The effect ZnO and GO on the structure, surface composition and photocatalytic activity of PVDF/GO/ZnO composite membranes were investigated. Owing to the strong hydrophilicity of the carboxyl group, the addition of GO enhanced the dispersibility of ZnO in PVDF membranes, which was proved by SEM results. Under Xenon irradiation (300 W), the photocatalytic degradation rate of PVDF/GO/ZnO composite membranes for methylene blue (MB) could reach 86.84%. Furthermore, the photocatalytic efficiency of the composites membrane for MB was evaluated with different initial concentrations of MB, pH value of the solution, and electron trapping agent-H2O2 content. And the radical trapping experiments with different active radical scavengers showed that the oxidizing species (O2-) plays an important role in the decolorization process of MB. In summary, this work provides an efficient method to improve the photodegradability of PVDF/GO/ZnO composite membranes and has great potential in the field of water purification.


Assuntos
Grafite/química , Membranas Artificiais , Azul de Metileno/química , Processos Fotoquímicos , Polivinil/química , Óxido de Zinco/química , Purificação da Água/métodos
3.
J Biomed Mater Res B Appl Biomater ; 106(8): 2869-2877, 2018 11.
Artigo em Inglês | MEDLINE | ID: mdl-29536617

RESUMO

Membrane surface design is significant for the development and application of synthetic polymer hemodialysis membranes. In this study, the influence of zwitterionic cysteine on poly(vinylidene fluoride) (PVDF) hollow fiber membrane was investigated. The polydopamine layer was formed through dopamine self-polymerization on PVDF membrane surface, and then cysteine was covalent grafted onto the layer to improve the anti-biofouling property and hemocompatibility. The elementary composition of membrane surfaces was characterized by X-ray photoelectron spectroscopy. The influence of polydopamine and cysteine on modified membrane surface morphologies was studied by field emission scanning electron microscopy. The modified PVDF membranes were confirmed to have excellent hydrophilicity, stable mechanical properties and good hemocompatibility (dynamic and static anti-protein adsorption, hemolysis ratio, plasma coagulation). And these properties were increased with the incorporation of polydopamine and cysteine. The optimized modified membranes exhibited high pure water flux (∼ 195.5 L/m2 h at 0.1 MPa) and selectivity (clearance ratio of urea and lysozyme was 75.1 and 55.4%, and rejection rate of bovine serum albumin was 98.8%). This work provides a surface modification method of PVDF hollow fiber membranes and suggests a potential application of PVDF membranes in hemodialysis field. © 2018 Wiley Periodicals, Inc. J Biomed Mater Res Part B: Appl Biomater, 106B: 2869-2877, 2018.


Assuntos
Materiais Revestidos Biocompatíveis/química , Cisteína/química , Indóis/química , Membranas Artificiais , Polímeros/química , Polivinil/química , Diálise Renal , Animais , Bovinos , Humanos , Teste de Materiais , Soroalbumina Bovina/química
4.
Biotechnol Appl Biochem ; 64(6): 888-894, 2017 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-27730684

RESUMO

Micro- and nanoimmunomagnetic beads (MIMBs and NIMBs) used for immunomagnetic separation (IMS) with PCR were studied for the rapid detection of Salmonella. The capture efficiency of the two different IMBs was evaluated by a conventional plate counting method, and the binding pattern was studied using scanning electron microscopy. The specificity of the IMBs was tested with Salmonella, Shigella flexneri, enterohemorrhagic Escherichia coli O157:H7, and Listeria monocytogenes. By comparing the pre-enrichment IMS and the IMS enrichment steps with a 5.5-H enrichment time, this study developed a rapid and sensitive method for the detection of Salmonella in chicken. The method was implemented by IMS enrichment and PCR with MIMBs and NIMBs, with a total analysis time of 8 H. We showed that the method was sensitive based on NIMBs with a detection limit of 10° CFU for Salmonella in 25 g of chicken.


Assuntos
Separação Imunomagnética , Reação em Cadeia da Polimerase , Salmonella/genética , Salmonella/isolamento & purificação , Animais , Galinhas , Separação Imunomagnética/instrumentação
5.
Mol Med Rep ; 15(1): 380-386, 2017 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-27959423

RESUMO

Gene expression data of hepatocellular carcinoma (HCC) was compared with that of cirrhosis (C) to identify critical genes in HCC. A total of five gene expression data sets were downloaded from Gene Expression Omnibus. HCC and healthy samples were combined as dataset HCC, whereas cirrhosis samples were included in dataset C. A network was constructed for dataset HCC with the package R for performing Weighted Gene Co­expression Network Analysis. Modules were identified by cluster analysis with the packages flashClust and dynamicTreeCut. Hub genes were screened out by calculating connectivity. Functional annotations were assigned to the hub genes using the Database for Annotation, Visualization and Integration Discovery, and functional annotation networks were visualized with Cytoscape. Following the exclusion of outlier samples, 394 HCC samples and 47 healthy samples were included in dataset HCC and 233 cirrhosis samples were included in dataset C. A total of 6 modules were identified in the weighted gene co­expression network of dataset HCC (blue, brown, turquoise, green, red and yellow). Modules blue, brown and turquoise had high preservation whereas module yellow exhibited the lowest preservation. These modules were associated with transcription, mitosis, cation transportation, cation homeostasis, secretion and regulation of cyclase activity. Various hub genes of module yellow were cytokines, including chemokine (C­C motif) ligand 22 and interleukin­19, which may be important in the development of HCC. Gene expression profiles of HCC were compared with those of cirrhosis and numerous critical genes were identified, which may contribute to the progression of HCC. Further studies on these genes may improve the understanding of HCC pathogenesis.


Assuntos
Carcinoma Hepatocelular/genética , Perfilação da Expressão Gênica , Regulação Neoplásica da Expressão Gênica , Neoplasias Hepáticas/genética , Carcinoma Hepatocelular/patologia , Análise por Conglomerados , Redes Reguladoras de Genes , Humanos , Fígado/patologia , Neoplasias Hepáticas/patologia , Transcriptoma
6.
Biomater Sci ; 4(11): 1673-1681, 2016 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-27709136

RESUMO

Our team has previously reported a high strength thermoplastic supramolecular polymer hydrogel. However, the hydrogel required injection temperatures outside the physiological range therefore preventing its use in a living environment. In this article, we reported a thermoresponsive supramolecular copolymer hydrogel p(N-acryloyl glycinamide-co-acrylamide) (PNAGA-PAAm), which can be injected at temperatures within the physiological range. We used rheological measurements to demonstrate that the transition temperature (upper critical solution temperature) of both the moduli and gel-sol could be finely adjusted by controlling both the ratio and concentration of the monomer. Adding iohexol (contrast agent) in PNAGA-PAAm hydrogels contributed to the decreased moduli and gel-sol transition temperature due to weakening of the hydrogen bonding interactions. The cytocompatible and hemocompatible PNAGA-PAAm sol mixed with iohexol was injected into the renal arteries of rabbits through a microcatheter at a temperature within the high biological range. The transition from the injection temperature (high biological range) to body temperature (basal for the animals) quickly solidified the embolic agent without the occurrence of dehydration, therefore overcoming the main limitation of LCST-typed poly(N-isopropylacrylamide) previously reported. Angiography and histological examination demonstrated the successful embolization of both renal arteries and no recanalization was observed after 8 weeks. The PNAGA-based supramolecular copolymer hydrogel is a novel embolic agent that allows for the occlusion of larger sized arteries in a biocompatible environment.


Assuntos
Artérias/efeitos dos fármacos , Embolização Terapêutica/métodos , Hidrogéis/farmacologia , Animais , Materiais Biocompatíveis/normas , Hidrogéis/química , Rim/irrigação sanguínea , Coelhos , Temperatura Ambiente
7.
Adv Mater ; 27(37): 5499-505, 2015 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-26270904

RESUMO

As nanotheranostics, Congo red/Rutin-MNPs combine the abilities of diagnosis and treatment of Alzheimer's disease (AD). The biocompatible nanotheranostics system based on iron oxide magnetic nanoparticles, with ultrasmall size and excellent magnetic properties, can specifically detect amyloid plaques by magnetic resonance imaging, realize targeted delivery of AD therapeutic agents, achieve drug controlled release by H2O2 response, and prevent oxidative stress.


Assuntos
Doença de Alzheimer/tratamento farmacológico , Doença de Alzheimer/patologia , Meios de Contraste , Portadores de Fármacos , Nanopartículas de Magnetita , Nanomedicina Teranóstica/métodos , Doença de Alzheimer/induzido quimicamente , Doença de Alzheimer/metabolismo , Precursor de Proteína beta-Amiloide/genética , Precursor de Proteína beta-Amiloide/metabolismo , Animais , Encéfalo/efeitos dos fármacos , Encéfalo/metabolismo , Encéfalo/patologia , Linhagem Celular Tumoral , Vermelho Congo/química , Meios de Contraste/química , Modelos Animais de Doenças , Portadores de Fármacos/química , Sistemas de Liberação de Medicamentos/métodos , Liberação Controlada de Fármacos , Compostos Férricos/química , Humanos , Peróxido de Hidrogênio/metabolismo , Imagem por Ressonância Magnética/métodos , Nanopartículas de Magnetita/química , Camundongos Transgênicos , Fármacos Neuroprotetores/administração & dosagem , Fármacos Neuroprotetores/química , Fármacos Neuroprotetores/farmacocinética , Estresse Oxidativo/efeitos dos fármacos , Estresse Oxidativo/fisiologia , Placa Amiloide/diagnóstico , Placa Amiloide/metabolismo , Placa Amiloide/patologia , Presenilina-1/genética , Presenilina-1/metabolismo , Rutina/administração & dosagem , Rutina/química , Rutina/farmacocinética
8.
Adv Mater ; 27(24): 3645-53, 2015 Jun 24.
Artigo em Inglês | MEDLINE | ID: mdl-25946668
9.
Theranostics ; 4(9): 904-18, 2014.
Artigo em Inglês | MEDLINE | ID: mdl-25057315

RESUMO

The controllable self-assembly of amphiphilic mixed polymers grafted gold nanoparitcles (AuNPs) leads to strong interparticle plasmonic coupling, which can be tuned to the near-infrared (NIR) region for enhanced photothermal therapy (PTT). In this study, an improved thiolation method was adopted for ATRP and ROP polymer to obtain amphiphilic brushes of PMEO2MA-SH and PCL-SH. By anchoring PCL-SH and PMEO2MA-SH onto the 14 nm AuNPs, a smart hybrid building block for self-assembly was obtained. Increasing the PCL/PMEO2MA chain ratio from 0.8:1, 2:1 and 3:1 to 7:1, the structure of gold assemblies (GAs) was observed to transfer from vesicle to large compound micelle (LCM). Contributed to the special dense packed structure of gold nanoparticles in LCM, the absorption spectrometry of gold nanoparticles drastically red-shifted from 520 nm to 830 nm, which endowed the GAs remarkable NIR photothermal conversion ability. In addition, gold has high X-ray absorption coefficient which qualifies gold nanomaterial a potential CT contrast agent Herein, we obtain a novel gold assembly structure which can be utilized as potential photothermal therapeutic and CT contrast agents. In vitro and In vivo studies testified the excellent treatment efficacy of optimum GAs as a PTT and CT contrast agent. In vitro degradation test, MTT assay and histology study indicated that GAs was a safe, low toxic reagent with good biodegradability. Therefore, the optimum GAs with strong NIR absorption and high X-ray absorption coefficient could be used as a theranostic agent and the formation of novel gold large compound micelle might offers a new theory foundation for engineering design and synthesis of polymer grafted AuNPs for biomedical applications.


Assuntos
Neoplasias Mamárias Experimentais/terapia , Nanopartículas Metálicas , Fototerapia , Tomografia Computadorizada por Raios X , Animais , Feminino , Ouro/química , Humanos , Células MCF-7 , Neoplasias Mamárias Experimentais/diagnóstico por imagem , Camundongos , Camundongos Endogâmicos BALB C , Camundongos Nus , Micelas
10.
J Control Release ; 176: 104-14, 2014 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-24365128

RESUMO

Cationic liposome based siRNA delivery system has improved the efficiencies of siRNA. However, cationic liposomes are prone to be rapidly cleared by the reticuloendothelial system (RES). Although modification of cationic liposomes with polyethylene glycol (PEG) could prolong circulation lifetime, PEG significantly inhibits siRNA entrapment efficiency, cellular uptake and endosomal/lysosomal escape process, resulting in low gene silencing efficiency of siRNA. In this study, we report the synthesis of zwitterionic polycarboxybetaine (PCB) based distearoyl phosphoethanolamine-polycarboxybetaine (DSPE-PCB) lipid for cationic liposome modification. The DSPE-PCB20 cationic liposome/siRNA complexes (lipoplexes) show an excellent stability in serum medium. The siRNA encapsulation efficiency of DSPE-PCB20 lipoplexes could reach 92% at N/P ratio of 20/1, but only 73% for DSPE-PEG lipoplexes. The zeta potential of DSPE-PCB20 lipoplexes is 8.19±0.53mV at pH 7.4, and increases to 24.6±0.87mV when the pH value is decreased to 4.5, which promotes the endosomal/lysosomal escape of siRNA. The DSPE-PCB20 modification could enhance the silencing efficiency of siRNA by approximately 20% over the DSPE-PEG 2000 lipoplexes at the same N/P ratio in vitro. Furthermore, DSPE-PCB20 lipoplexes could efficiently mediate the down-regulation of Apolipoprotein B (ApoB) mRNA in the liver and consequently decrease the total cholesterol in the serum in vivo, suggesting therapeutic potentials for siRNA delivery in hypercholesterolemia-related diseases.


Assuntos
Betaína/química , Fosfatidiletanolaminas/química , RNA Interferente Pequeno/administração & dosagem , Animais , Apolipoproteínas B/genética , Sobrevivência Celular , Endossomos/metabolismo , Células HeLa , Humanos , Lipossomos , Fígado/metabolismo , Luciferases/genética , Luciferases/metabolismo , Lisossomos/metabolismo , Masculino , Camundongos , Camundongos Endogâmicos C57BL , Polietilenoglicóis/química , RNA Mensageiro/metabolismo
11.
J Biomater Sci Polym Ed ; 24(3): 330-43, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-23565651

RESUMO

Cationic polyplexes would aggregate immediately after intravenous injection due to the plasma proteins and high ionic strength. A cationic polyplexes with long-term and salt stability was very important for a systemic gene therapy. In this research, a polysulfobetaine-b-polycation diblock copolymer composed of cationic block of poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) and zwtterionic block of poly(propylsulfonate dimethylammonium ethylmethacrylate) (PSPE) was conveniently synthesized by atom transfer radical polymerization method to obtain a cationic polymers with long-term and salt stability. The results of agarose gel electrophoresis and transmission electron microscope indicated that copolymerization of PSPE did not compromise the DNA condensation ability of PDMAEMA, meanwhile exhibiting lower cytotoxicity. The effect of salt on the absorbance and particle size of PDMAEMA100/DNA and PDMAEMA100-PSPEy/DNA complexes was investigated, which showed that PSPE block could increase the resistance of polyplexes against salt-induced aggregation owing to the antielectrolyte effect. In comparison with PDMAEMA homopolymer, PDMAEMA100-PSPEy retained more stable gene transfection in a certain range of salt concentration. The expression of red fluorescence protein (RFP) was evaluated by small animal in vivo fluorescence imaging system and the results showed that the expression of RFP was much higher in the mice injected with PDMAEMA100-PSPE20/pDNA-RFP than with PDMAEMA/pDNA-RFP. Both in vitro and in vivo results suggested that PDMAEMA-PSPE diblock copolymer may be potentially used as a vector for systemic gene therapy.


Assuntos
Betaína/análogos & derivados , Metacrilatos/química , Metacrilatos/metabolismo , Nylons/química , Nylons/metabolismo , Sais/química , Transfecção/métodos , Animais , Betaína/química , Células COS , Fenômenos Químicos , DNA/genética , Masculino , Metacrilatos/toxicidade , Camundongos , Camundongos Nus , Nylons/toxicidade
12.
Biomaterials ; 32(2): 628-38, 2011 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-20888634

RESUMO

Polyethylene glycol or phosphorylcholine is often introduced into polycationic non-viral vectors to inhibit the non-specific protein adsorption. However the ability of vectors to condense DNA and the cellular internalization of complexes are unavoidably compromised. In this work, a polysulfobetaine-cationic methacrylate copolymer: 2-(dimethylamino) ethyl methacrylate-block-(N-(3-(methacryloylamino) propyl)-N,N-dimethyl-N-(3-sulfopropyl) ammonium hydroxide) (PDMAEMA-b-PMPDSAH) diblock copolymer was synthesized via atomic transfer radical polymerization method and investigated as a new non-viral vector for gene delivery. Incorporation of polysulfobetaine into cationic methacrylate retained a better DNA condensation capability. MTT assays revealed that the cytotoxicity of PDMAEMA(200)-PMPDSAH(n) copolymer was lower than that of PDMAEMA(200). PDMAEMA(200)-PMPDSAH(80) which was much superior to its homopolymer in mediating gene transfection demonstrated comparable efficiency to PEI25 kDa at a weight ratio of 8 in the presence of 10% serum. At higher serum contents, the transfection of PDMAEMA(200) and PEI25 kDa was deteriorated, whereas PDMAEMA(200)-PMPDSAH(80) still retained better transfection efficiency, 4-5 fold more effective than PEI25 kDa. For the sake of comparative study, we synthesized structurally similar copolymer from DMAEMA and 2-methacryloyloxyethyl phosphorylcholine, PDMAEMA(200)-PMPC(80). PDMAEMA(200)-PMPDSAH(80) exhibited much higher gene transfer levels than PDMAEMA(200)-PMPC(80) under the same conditions. The results of flow cytometry indicated that highly hydrophilic MPC block profoundly impeded the cellular internalization of nanocomplexes; in contrast, incorporation of polysulfobetaine remained the increased cellular uptake. Differential scanning calorimetry assay of thermodynamic phase transition of dipalmitoyl-sn-glycero-3-phosphocholine(DPPC) induced by polymer vectors demonstrated that MPC only marginally contributed to the perturbation of DPPC; polysulfobetaine facilitated more evident perturbation of DPPC bilayer instead, an indication that polysulfobetaine units could aid in the endocytosis of nanocomplexes.


Assuntos
Betaína/análogos & derivados , Betaína/química , Vetores Genéticos/química , Metacrilatos/química , Nylons/química , Polímeros/química , Transfecção/métodos , Animais , Células COS , Varredura Diferencial de Calorimetria
13.
Biomaterials ; 31(3): 559-69, 2010 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-19796806

RESUMO

In this work, we synthesized a star cationic polymer(s-PDMAEMA) consisting of cleavable poly[N,N-bis(acryloyl) cystamine](PBAC) crosslinked core and poly(N,N-dimethyl-ethylamine methacrylate) (PDMAEMA) arms by atomic transfer radical polymerization using one-pot "arm first" method. The s-PDMAEMA that was degradable in a mimic intracellular redox environment was more efficient in condensing DNA. It was shown that s-PDMAEMA achieved higher gene transfection levels relative to their linear precursors and s-PDMAEMA200 with longer and more arms exhibited superior transfection efficiencies and lower cytotoxicity compared to PEI25K. The buffer capacities were examined by acid-base titration; the pH-dependent morphological evolution and enzyme stability of PDMAEMA/DNA complexes were investigated by atomic force microscopy (AFM) and time-resolved fluorescence spectroscopy, respectively. The results indicated that the star polymers exhibited a stronger buffering ability than their linear precursors due to the increased inner osmotic pressure. By decreasing the pH from 7.4 to 5.0, the linear PDMEMA/DNA complexes became more compact; in contrast, s-PDMAEMA200/DNA complex adopted a loose morphology due to the steric barrier of inter-arms and outward extension of positively charged arms. Analysis of the fluorescence life times of free and intercalated ethidium bromide unveiled more effective protection of DNA afforded by s-PDMAEMA. The effect of medium pH on the star PDMAEMA system was smaller owing to the ability of densely tertiary amino groups along multiple arms to absorb more protons, which was favorable for endosomolytic escape of complexes.


Assuntos
Técnicas de Transferência de Genes , Vetores Genéticos/metabolismo , Metacrilatos , Nylons , Animais , Linhagem Celular , Reagentes para Ligações Cruzadas/química , Dissulfetos/química , Endossomos/metabolismo , Humanos , Concentração de Íons de Hidrogênio , Lisossomos/metabolismo , Teste de Materiais , Metacrilatos/síntese química , Metacrilatos/química , Microscopia de Força Atômica , Estrutura Molecular , Peso Molecular , Nylons/síntese química , Nylons/química , Oxirredução
14.
J Mater Sci Mater Med ; 20(4): 967-74, 2009 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-19020956

RESUMO

Thermoresponsive BAB-type HEMA/NIPAAm triblock copolymers (A = NIPAAm, B = HEMA) were prepared by atomic transfer radical polymerization (ATRP). BAB1-6 with shorter PNIPAAm blocks failed to form stable gel; while a relatively stable gel could be achieved by BAB1-8 with longer PNIPAAm blocks when copolymer aqueous solution was heated up. Introducing radiopaque agent (RA) was shown to slightly increase the transition temperature and gelation time, but the gelling ability was strengthened due to slightly weakening dehydration of copolymer in the mixture of water and RA. BAB1-8 aqueous solution about 5 wt% in the presence of RA was demonstrated to successfully occlude the cerebral rete mirabiles (RMs) and renal arteries of pigs. Within 3-month surgery, no recanalization was observed and the embolized kidney shrank considerably. Histological assay of embolized kidney demonstrated interstitial fibrosis and calcification as well as the thickening of renal small artery. This temperature sensitive copolymer with well-defined architecture holds a great potential as an embolic agent for treating arteriovenous malformations (AVMs) and renal disease due to the design flexibility of ATRP.


Assuntos
Resinas Acrílicas/química , Malformações Arteriovenosas/terapia , Embolização Terapêutica , Metacrilatos/química , Animais , Varredura Diferencial de Calorimetria , Feminino , Masculino , Reologia , Soluções , Suínos , Porco Miniatura
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