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1.
Nanoscale ; 12(19): 10426-10429, 2020 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-32393940
2.
Langmuir ; 2020 May 27.
Artigo em Inglês | MEDLINE | ID: mdl-32407120

RESUMO

Precise control over on-surface covalent reaction pathways is crucial for engineering organic nanostructures with the single-atom precision. Herein, we demonstrate a step-by-step control of an on-surface cascade covalent reaction based on a successive debromination templated by noncovalent metal-organic coordination motifs. The molecular precursor is predesigned with different reactive sites and functional ligands, allowing for both chemical and structural tuning during on-surface reactions. Through the Fe-terpyridine template effect, we are able to direct the reaction to proceed in a three-step cascade pathway and finally to achieve a porous polyarylene nanoribbon structure. The approach opens new opportunities for construction of on-surface organic nanostructures in a predictable manner.

3.
Langmuir ; 2020 Apr 06.
Artigo em Inglês | MEDLINE | ID: mdl-32216353

RESUMO

The self-assembly of oppositely charged colloidal ellipsoids and spheres under active confinement is first proposed to achieve long-range ordered photonic crystals. Compared with the conventional passive confinement, a characteristic of the active confinement is that boundaries are movable. Our Brownian dynamics simulations show that dynamic steady structures, similar to quasi-2D colloidal crystals, can be obtained under the strong confinement when the two boundaries periodically oscillate together. The in-plane structures can be regulated by changing the charge ratio of the two kinds of particles. These dynamic steady structures are determined by the minimum electrostatic energy with the aid of increased mobility of confined particles, which are not available in equilibrium. Numerical simulations verify that light can be perfectly confined in this dielectric binary photonic slab without any radiation, which corresponds to a typical optical bound state with divergent lifetime and ultrasharp spectral profile. Given the changeable geometry of this photonic slab, the trapped optical field might be applicable to enhanced light-matter interactions. In addition, for thicker layers, layer-by-layer ordered structures occur spontaneously, driven by the active confinement, while no global order occurs in the passive confinement. Our results show that the boundary motion can become an important factor affecting self-assembled structure and function.

4.
Nanoscale ; 12(14): 7804-7813, 2020 Apr 14.
Artigo em Inglês | MEDLINE | ID: mdl-32219265

RESUMO

It is important to maintain the balance between therapeutic efficiency and cytotoxicity when using nanomaterials for biomedical applications. Here, we propose a new method (i.e., non-covalent coating of protected copolymers onto the nanoparticle surface) to enhance the active targeting of nanoparticles to the cancer cells by combining the dissipative particle dynamics simulation and in vitro experiments. When coating the protected copolymer onto the nanoparticle surface, the uptake efficiency could be greatly altered due to the competition between the copolymer-ligand interaction and the receptor-ligand interaction-the non-covalent coating is more efficient than the covalent coating. Furthermore, the effect of the physicochemical properties of the protected copolymer on the targeting ability of nanoparticles was also investigated. This study offers useful insight into the optimal design of nanocarriers in biomedicine.

5.
J Am Chem Soc ; 142(10): 4800-4806, 2020 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-32049531

RESUMO

The ubiquitous biomembrane interface, with its dynamic lateral fluidity, allows membrane-bound components to rearrange and localize for high-affinity multivalent ligand-receptor interactions in diverse life activities. Inspired by this, we herein engineered a fluidic multivalent nanointerface by decorating a microfluidic chip with aptamer-functionalized leukocyte membrane nanovesicles for high-performance isolation of circulating tumor cells (CTCs). This fluidic biomimetic nanointerface with active recruitment-binding afforded significant affinity enhancement by 4 orders of magnitude, exhibiting 7-fold higher capture efficiency compared to a monovalent aptamer functionalized-chip in blood. Meanwhile, this soft nanointerface inherited the biological benefits of a natural biomembrane, minimizing background blood cell adsorption and maintaining excellent CTC viability (97.6%). Using the chip, CTCs were successfully detected in all cancer patient samples tested (17/17), suggesting the high potential of this fluidity-enhanced multivalent binding strategy in clinical applications. We expect this bioengineered interface strategy will lead to the design of innovative biomimetic platforms in the biomedical field by leveraging natural cell-cell interaction with a natural biomaterial.

6.
Colloids Surf B Biointerfaces ; 188: 110755, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-31887646

RESUMO

Natural cellular membranes, with the outstanding qualities of biocompatibility and specificity, have gained growing attentions in the system of drug delivery. Nanoparticles coated with cellular membranes are starting to be applied as drug-loaded-vehicles to target tumors. Here, neutrophil membranes were selected to apply in the treatment of inflammation because neutrophils can participate in various inflammatory responses and accumulate at inflammatory sites to eliminate pathogens. Through extracting neutrophil membranes from natural neutrophils without affecting their biological properties, nanoparticles loaded with sparfloxacin (SPX) were coated with these membranes and disguised as neutrophils. Compared with traditional nano-medicines, the neutrophil membrane-coated nanoparticles (NM-NP-SPX) possessed precise targeting ability just like the neutrophils could accumulate at inflammatory sites when inflammation burst. In addition, NM-NP-SPX could prolong the circulation time and had the property of controlled-release. Through in vivo experiments, we found that the concentration of three representative inflammatory cytokines in blood, bacteria and inflammatory cells in lungs of the mice with pneumonia reduced significantly in the initial 24 h after the injection of NM-NP-SPX, which meant that NM-NP-SPX could greatly reduce the risk of death for the patients with inflammation. Moreover, the infected lungs could recover rapidly without any side effects to other organs due to the low cytotoxicity of NM-NP-SPX against normal cells. Therefore, our developed drug delivery system has enormous advantages in treating inflammations. Not only that, this kind of bionic method may have greater value and application prospects in curing the inflammations arisen from cancers.

7.
J Am Chem Soc ; 141(47): 18910-18915, 2019 Nov 27.
Artigo em Inglês | MEDLINE | ID: mdl-31691568

RESUMO

Receptor-ligand interactions (RLIs) that play pivotal roles in living organisms are often depicted with the classic keys-and-locks model. Nevertheless, RLIs on the cell surface are generally highly complex and nonlinear, partially due to the noncontinuous and dynamic distribution of receptors on extracellular membranes. Here, we develop a tetrahedral DNA framework (TDF)-programmed approach to topologically engineer RLIs on the cell membrane, which enables active recruitment-binding of clustered receptors for high-affinity capture of circulating tumor cells (CTCs). The four vertices of a TDF afford orthogonal anchoring of ligands with spatial organization, based on which we synthesized n-simplexes harboring 1-3 aptamers targeting epithelial cell adhesion molecule (EpCAM) that are overexpressed on the membrane of tumor cells. The 2-simplex with three aptamers not only shows increased binding affinity (∼19-fold) but prevents endocytosis by cells. By using 2-simplex as the capture probe, we demonstrate the high-efficiency CTC capture, which is challenged in real clinical breast cancer patient samples. This TDF-programmed platform thus provides a powerful means for studying RLIs in physiological settings and for cancer diagnosis.

8.
Nat Commun ; 10(1): 4520, 2019 10 04.
Artigo em Inglês | MEDLINE | ID: mdl-31586045

RESUMO

Control over the protein corona of nanomaterials allows them to function better. Here, by taking graphene/gold as examples, we comprehensively assessed the association of surface properties with the protein corona. As revealed by in vitro measurements and computations, the interaction between graphene/gold and HSA/IgE was inversely correlated with the hydroxyl group availability, whereas the interaction between that and ApoE was comparatively less relevant. Molecular simulations revealed that the number and the distribution of surface hydroxyl groups could regulate the manner in which nanomaterials interact with proteins. Moreover, we validated that ApoE pre-adsorption before injection enhances the blood circulation of nanomaterials relative to their pristine and IgE-coated counterparts. This benefit can be attributed to the invulnerability of the complementary system provided by ApoE, whose encasement does not increase cytotoxicity. Overall, this study offers a robust yet simple way to create protein corona enriched in dysopsonins to realize better delivery efficacy.


Assuntos
Portadores de Fármacos/química , Nanopartículas/química , Coroa de Proteína/metabolismo , Adsorção , Animais , Apolipoproteínas E/química , Apolipoproteínas E/metabolismo , Linhagem Celular Tumoral/transplante , Modelos Animais de Doenças , Portadores de Fármacos/administração & dosagem , Portadores de Fármacos/farmacocinética , Feminino , Ouro/química , Grafite/química , Humanos , Imunoglobulina E/química , Imunoglobulina E/metabolismo , Injeções Intravenosas , Camundongos , Simulação de Dinâmica Molecular , Nanopartículas/metabolismo , Neoplasias/tratamento farmacológico , Proteínas Opsonizantes/química , Ligação Proteica , Coroa de Proteína/química , Estrutura Secundária de Proteína , Células RAW 264.7 , Albumina Sérica Humana/metabolismo , Propriedades de Superfície
9.
Langmuir ; 35(39): 12851-12857, 2019 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-31474103

RESUMO

The well control over the cell-nanoparticle interaction can be of great importance and necessity for different biomedical applications. In this work, we propose a new and simple way (i.e., polymeric tether) to tuning the interaction between nanoparticles and cell membranes by dissipative particle dynamics simulations. It is found that the linked nanoparticles (via polymeric tether) can show some cooperation during the cellular uptake and thereby have a higher wrapping degree than the single nanoparticle. The effect of the property of the polymer on the wrapping is also investigated, and it is found that the length, rigidity, and hydrophobicity of the polymer play an important role. More interestingly, the uptake of linked nanoparticles could be adjusted to the firm adhesion via two rigid polymeric tethers. The present study may provide some useful guidelines for novel design of functional nanomaterials in the experiments.

10.
Adv Healthc Mater ; 8(9): e1801521, 2019 05.
Artigo em Inglês | MEDLINE | ID: mdl-30866165

RESUMO

Antimicrobial peptides (AMPs) promise a fundamental solution to the devastating threat of drug-resistant bacteria. However, drawbacks of AMPs (e.g., poor cell membrane penetration efficiency) seriously block their clinical use. In this work, rational design of a hybrid complex of melittin (as a representative AMP) and graphene or graphene oxide (Gra or GO) nanosheets for enhanced antibacterial ability is achieved, via combining in-silico prediction and in-tube test. In comparison to pristine melittin, the specifically designed AMP-Gra (/GO) complex exhibits remarkable efficiency in transmembrane perforation with an over tenfold decrease in the threshold working concentration of peptide; moreover, it has an up to 20-fold enhancement in antibacterial activity against both Gram-negative and Gram-positive bacteria. Such improvement is ascribed to the synergetic insertion of nanosheets and melittin due to similarity in antibacterial mechanism between them and is further regulated by the structural factors of the complex, including the intersheet spacing and surface functionalization of the Gra/GO sheets, etc. These results provide practical guidelines to engineer AMPs with nanotechnology for improved antimicrobial performances, especially based on targeted functionalization of the Gra/GO nanosheets.

11.
Phys Chem Chem Phys ; 21(8): 4487-4493, 2019 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-30734786

RESUMO

Folding and unfolding of a chain structure are often manipulated in experiments by tuning the pH, temperature, single-molecule forces or shear fields. Here, we carry out Brownian dynamics simulations to explore the behavior of a single self-attracting chain in a suspension of self-propelling particles (SPPs). As the propelling force increases, the globule-stretch (G-S) transition of the chain occurs due to the enhanced disturbance from the SPPs. Two distinct mechanisms of the transition in the limits of low and high rotational diffusion rates of SPPs have been observed: shear-induced stretching at a low rate and collision-induced melting at a high rate. The G-S and S-G (stretch-globule) curves form a hysteresis loop at the low rate, while they merge at the high rate. Besides, we find that two competing effects result in a non-monotonic dependence of the G-S transition on SPP density at the low rate. Our results suggest an alternative approach to manipulating the folding and unfolding of (bio)polymers by utilizing active agents.

12.
Phys Rev E ; 99(1-1): 010601, 2019 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-30780307

RESUMO

We show that the dominant mode of alignment plays an important role in dry active nematics, leading to two dynamical subclasses defined by the nature of the instability of the nematic bands that characterize, in these systems, the coexistence phase separating the isotropic and fluctuating nematic states. In addition to the well-known instability inducing long undulations along the band, another stronger instability leading to the breakup of the band in many transversal segments may arise. We elucidate the origin of this strong instability for a realistic model of self-propelled rods and determine the high-order nonlinear terms responsible for it at the hydrodynamic level.

13.
Nat Commun ; 10(1): 70, 2019 01 08.
Artigo em Inglês | MEDLINE | ID: mdl-30622253

RESUMO

Control over on-surface reaction pathways is crucial but challenging for the precise construction of conjugated nanostructures at the atomic level. Herein we demonstrate a selective on-surface covalent coupling reaction that is templated by metal-organic coordinative bonding, and achieve a porous nitrogen-doped carbon nanoribbon structure. In contrast to the inhomogeneous polymorphic structures resulting from the debrominated aryl-aryl coupling reaction on Au(111), the incorporation of an Fe-terpyridine (tpy) coordination motif into the on-surface reaction controls the molecular conformation, guides the reaction pathway, and finally yields pure organic sexipyridine-p-phenylene nanoribbons. Emergent molecular conformers and reaction products in the reaction pathways are revealed by scanning tunneling microscopy, density functional theory calculations and X-ray photoelectron spectroscopy, demonstrating the template effect of Fe-tpy coordination on the on-surface covalent coupling. Our approach opens an avenue for the rational design and synthesis of functional conjugated nanomaterials with atomic precision.

14.
Nanoscale ; 11(5): 2170-2178, 2019 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-30376020

RESUMO

Efficient and accurate detection of cancer cells (from normal cells) is of great importance in cancer diagnosis and prognosis. In this work, we design a new type of polymeric substrate containing nanoparticles for detecting cancers by the dissipative particle dynamics (DPD) simulation. It is found that the cancer cells and the normal cells can be indeed distinguished since the uptake number of nanoparticles from the substrate is different. The competition between the nanoparticle-cell specific interaction and nanoparticle-polymer non-specific interaction is the main factor for different uptake behaviors. Moreover, the dynamics of the nanoparticle diffusion in the polymer layer also plays an important role in the detection. To improve the detection accuracy, we further investigate the effect of the polymer type and density as well as the ligand type on the detection, and find that there may exist an optimal parameter to maximize the difference between cancer cells and normal cells. The present study may provide useful insights into the design of functionalized substrate-based nanodevices in biomedicine.


Assuntos
Simulação por Computador , Nanopartículas/química , Neoplasias/diagnóstico , Neoplasias/patologia , Polímeros/química , Transporte Biológico , Membrana Celular/metabolismo , Difusão , Humanos , Ligantes , Modelos Moleculares , Software
15.
Phys Chem Chem Phys ; 20(44): 28241-28248, 2018 Nov 14.
Artigo em Inglês | MEDLINE | ID: mdl-30398246

RESUMO

Cell membrane-based sorting and trafficking of nanoscale particles (NPs) are fundamental processes in many cellular activities such as endocytosis, signaling and virus infection; however, the regulation mechanism of these behaviors is still poorly understood. In this work, partitioning of NPs into different lipid phases (i.e., liquid-ordered and liquid-disordered phases) on a ternary lipid bilayer, as well as the influence of NP perturbations on the phase separation of the bilayer, is investigated by using coarse-grained molecular dynamics simulations. Interestingly, it is revealed by our simulations that even with the same chemical affinity between the NPs and lipids in different phases, NPs are still able to preferentially locate at the liquid-disordered (Ld) phase domains. The preferential partitioning behavior of NPs is associated with the physical properties of both the membrane and NPs (e.g., the membrane stiffness and the NP size/quantity). Additionally, the preferential partitioning of NPs facilitates growth of the Ld domain and promotes coupling of this domain between the two leaflets. This work provides new insights into the complicated nano-bio interaction mechanism. Moreover, it suggests methods to regulate the mobility of NPs on cellular membranes to modulate important biological processes accordingly.


Assuntos
Bicamadas Lipídicas/química , Simulação de Dinâmica Molecular , Nanopartículas/química , Transporte Biológico , Fenômenos Biomecânicos , Membrana Celular/química , Cinética , Lipídeos/química , Tamanho da Partícula , Propriedades de Superfície , Termodinâmica
16.
ACS Cent Sci ; 4(10): 1344-1351, 2018 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-30410972

RESUMO

Cell entry of anionic nano-objects has been observed in various types of viruses and self-assembled DNA nanostructures. Nevertheless, the physical mechanism underlying the internalization of these anionic particles across the negatively charged cell membrane remains poorly understood. Here, we report the use of virus-mimicking designer DNA nanostructures with near-atomic resolution to program "like-charge attraction" at the interface of cytoplasmic membranes. Single-particle tracking shows that cellular internalization of tetrahedral DNA nanostructures (TDNs) depends primarily on the lipid-raft-mediated pathway, where caveolin plays a key role in providing the short-range attraction at the membrane interface. Both simulation and experimental data establish that TDNs approach the membrane primarily with their corners to minimize electrostatic repulsion, and that they induce uneven charge redistribution in the membrane under the short-distance confinement by caveolin. We expect that the nanoscale like-charge attraction mechanism provides new clues for viral entry and general rules for rational design of anionic carriers for therapeutics.

17.
Biochim Biophys Acta Biomembr ; 1860(11): 2234-2241, 2018 11.
Artigo em Inglês | MEDLINE | ID: mdl-30409519

RESUMO

Antimicrobial peptides (AMPs) provide a promising solution to the serious threat of multidrug-resistant bacteria or superbugs to public healthcare, due to their unique disruption to bacterial membrane such as perforation. Unfortunately, the underlying action mechanism of AMPs, especially the possible transition between the membrane binding and perforation states of peptides (i.e., the classical two-state model), is still largely unknown. Herein, by combining experimental techniques with pertinent membrane models and molecular dynamic (MD) simulations, new insights into the intermediate states of the AMP melittin-membrane interaction process are obtained. Specifically, it is demonstrated that, after the initial binding, the accumulated melittin on the bilayer triggers vigorous fluctuation of the membrane and even extracts some lipid molecules exclusively from the deformed outer leaflet of the bilayer. Such a distinctive mass removal manner and the resultant local asymmetry in lipid number between the two leaflets change the mechanical status of the membrane and in turn reduce the free energy barrier for the melittin insertion. Finally, the formation of the transmembrane pores is facilitated significantly. These findings provide new insights into the complicated antimicrobial mechanisms of AMPs.


Assuntos
Anti-Infecciosos/farmacologia , Meliteno/farmacologia , Membrana Celular/efeitos dos fármacos , Bicamadas Lipídicas/metabolismo , Simulação de Dinâmica Molecular , Peptídeos/química , Peptídeos/farmacologia , Técnicas de Microbalança de Cristal de Quartzo
18.
J Chem Phys ; 149(16): 164902, 2018 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-30384734

RESUMO

In an earlier work, we discussed the possibility to realize a microrotor by immersing a chain-grafted colloidal disk in a thin film of active-particle suspension. Under certain conditions, the colloidal disk rotates unidirectionally driven by the bath active particles. Here we systematically study the role of active-particle concentration, grafting density, and chain rigidity in the phenomenon of the spontaneous symmetry breaking of the chain configurations and the unidirectional rotation of the disk. We find that high chain rigidity can help stabilize both the collective asymmetric chain configurations and the rotation of the disk, while it has a weak impact on the rotational speed/efficiency. Increasing the number of grafted chains can also stabilize the rotation but has a negative impact on the rotational speed/efficiency. Active particles power the rotation of the colloidal disk, yet their contribution saturates beyond a certain concentration. Our work provides new insights into the active systems with chain-structured objects and the design of soft/deformable micromachines.

19.
Inorg Chem ; 57(19): 12143-12154, 2018 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-30226764

RESUMO

Four pairs of enantiomeric dysprosium(III) phosphonates, namely, R- or S-[Dy3(pempH2)2(pempH)7]2(NO3)4·12H2O ( R-1 or S-1), R- or S-[Dy3(pempH)7(pempH2)2]Cl2·2H2O ( R-2 or S-2), R- or S-[Dy3(pempH)7(pempH2)2]Br2·2H2O ( R-3 or S-3), and R- or S-[Dy11(pempH2)6(pempH)27](CF3SO3)6·22H2O ( R-4 or S-4) are reported, where R- or S-pempH2 represent R- or S-(1-phenylethyl)amino] methylphosphonic acid. All show homochiral chain structures, charge-balanced by counteranions. A comparison of the crystal morphologies of the R-isomers reveals that the overall shapes are quite similar for the four compounds, but the aspect ratio changes remarkably following the sequence: R-1 < R-2 < R-3 < R-4. The sequence is in agreement with the decreasing interchain interactions related to different counteranions, which is rationalized by molecular simulations. The counteranions also influence the intrachain structures and the local coordination environments of the DyIII ions. As a result, compounds R-2 and R-3 exhibit distinct dual relaxation processes at zero dc field with the effective energy barriers for the slow- and fast-relaxation being 79.1 and 37.6 K for R-2, and 80.0 and 39.1 K for R-3, respectively. For compounds R-1 and R-4, however, slow magnetic relaxation is also observed at zero dc field but without the appearance of maxima down to 1.8 K.

20.
Langmuir ; 34(33): 9829-9835, 2018 08 21.
Artigo em Inglês | MEDLINE | ID: mdl-30056705

RESUMO

The efficient capture of nanoscopic particulates plays a key role in many scientific fields like filtration and fabrication of nanocomposites as well as biosensors. In this work, we design two types of nanosubstrates to capture the nanoparticle with specific property by using Brownian dynamics simulations. It is found that the substrate coated with copolymers (composed of nonspecific block and specific block) can be used to capture the nanoparticle with different sizes but its capture efficiency of nanoparticles with different shapes is very low. To overcome such problem, the other substrate containing shaped holes is also designed. By conducting a serial of control simulations, we find that the nonspecific polymers at the bottom and on the rim of the hole have great impact on the sensitive capture. The present study may provide some physical insights into the experimental design of nanodevices in real applications.

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