ORCID Profile
0000-0003-1018-4336
Current Organisation
Shandong University
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Publisher: Elsevier BV
Date: 02-2009
DOI: 10.1016/J.JCIS.2008.10.075
Abstract: Magnetic nanocapsules were constructed by fabricating nanometer scaled C(60)-like "Keplerate" type {Mo(72)Fe(30)} with molecular formula [Mo(72)(VI)Fe(30)(III)O(252)(CH(3)COO)(12){Mo(2)O(7)(H(2)O)}(2){H(2)Mo(2)O(8)(H(2)O)}(H(2)O)(91)] x ca.150 H(2)O into nanocapsule shells using the LbL technique. The morphology of the obtained hybrid nanocapsules was examined by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Shell thickness of the {Mo(72)Fe(30)}-embedded nanocapsules can be tailored at the nanometer level more precisely than other nanoparticle-embedded capsules due to the homogeneous diameter and surface charges of {Mo(72)Fe(30)}. Interestingly, the {Mo(72)Fe(30)}-embedded nanocapsules could be separated and aligned under a circumstance of magnetic field, though {Mo(72)Fe(30)} is a paramagnetic molecule. This is the first time to fabricate hybrid magnetic materials containing {Mo(72)Fe(30)} using LbL technique. The obtained nanocapsules can be a good candidate for bioseparation as well as targeted delivery.
Publisher: American Chemical Society (ACS)
Date: 02-11-2012
DOI: 10.1021/NN3039353
Abstract: We report a versatile approach for controlling the intracellular degradation of polymer capsules by tailoring the degree of cross-linking in the capsules. Poly(2-diisopropylaminoethyl methacrylate) capsules were assembled by the layer-by-layer technique and covalently stabilized with a redox-responsive bisazide cross-linker using click chemistry. The degree of cross-linking, determined using radiation scintillation counting, was tuned from 65% to 98% by adjusting the amount of cross-linker used to stabilize the polymer films. Transmission electron microscopy and fluorescence microscopy studies showed that the pH responsiveness of the capsules was maintained, regardless of the degree of cross-linking. Atomic force microscopy measurements on planar surfaces revealed that increasing the degree of cross-linking decreased the film roughness (from 8.7 to 1.7 nm), hence forming smoother films however the film thicknesses were not significantly altered. Cellular studies showed that the rate of intracellular degradation of the capsules could be controlled between 0 and 6 h by altering the degree of cross-linking in the polymer capsules. These studies also demonstrated that the cellular degradation of highly cross-linked capsules (>90%) was significantly retarded compared to degradation in simulated cellular conditions. This suggests that the naturally occurring cellular reducing environment is rapidly depleted, and there is a significant delay before the cells can replenish the reducing environment. The modular and versatile nature of this approach lends itself to application to a wide range of polymer carriers and thus offers significant potential for the design of polymer-based systems for drug and gene delivery.
Publisher: American Chemical Society (ACS)
Date: 02-03-2021
Publisher: American Chemical Society (ACS)
Date: 27-08-2009
DOI: 10.1021/CM901621Y
Publisher: American Chemical Society (ACS)
Date: 23-10-2023
Publisher: Wiley
Date: 04-04-2014
Abstract: A new class of polymer capsules with an in-built endocytic pH-coupled fluorescence switch is reported. These capsules display reversible "on/off" fluorescence in response to cellular pH variations. Using this system, the high-throughput quantification between surface-bound and internalized capsules is demonstrated. This system allows a fundamental study of the interaction between nanoengineered materials and biological systems at a cellular level.
Publisher: Wiley
Date: 12-07-2012
Publisher: Wiley
Date: 25-08-2021
Abstract: We report a sono‐Fenton strategy to mediate the supramolecular assembly of metal–phenolic networks (MPNs) as substrate‐independent coatings using phenol and phenyl derivatives as building blocks. The assembly process is initiated from the generation of hydroxyl radicals ( . OH) using high‐frequency ultrasound (412 kHz), while the metal ions synergistically participate in the production of additional . OH for hydroxylation henolation of phenol and phenyl derivatives via the Fenton reaction and also coordinate with the phenolic compounds for film formation. The coating strategy is applicable to various phenol and phenyl derivatives and different metal ions including Fe II , Fe III , Cu II , and Co II . In addition, the sono‐Fenton strategy allows real‐time control over the assembly process by turning the high‐frequency ultrasound on or off. The properties of the building blocks are maintained in the formed films. This work provides an environmentally friendly and controllable method to expand the application of phenolic coatings for surface engineering.
Publisher: American Chemical Society (ACS)
Date: 09-12-2019
DOI: 10.1021/ACS.LANGMUIR.9B03107
Abstract: We report the fabrication of polymer nanogels with a pH-responsive core and a pH-sheddable shell and investigate the pH-dependent cell association of the pH-responsive polymer nanogels. The pH-responsive core composed of poly(2-diisopropylaminoethyl methacrylate) (PDPA) with a p
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CC04938D
Abstract: Polyethylene glycol (PEG) has been widely used for modifying surfaces to reduce non-specific interactions with biomolecules, microorganisms, and cells. Herein, we report a sticktight-inspired PEGylation strategy to fabricate low-fouling coatings. The influence of PEG molecular architectures on the PEG density and biological adhesion were studied. Notably, an increase in the number of arms resulted in improved surface PEGylation and an improved antifouling ability against the adhesion of proteins, mammalian cells and bacteria. The molecular architecture-dependent PEGylation strategy is an attractive approach for developing advanced low-fouling coatings.
Publisher: American Chemical Society (ACS)
Date: 31-10-2014
DOI: 10.1021/BM5012272
Abstract: We report the preparation of polymer-peptide blend replica particles via the mesoporous silica (MS) templated assembly of poly(ethylene glycol)-block-poly(2-diisopropylaminoethyl methacrylate-co-2-(2-(2-(prop-2-ynyloxy)ethoxy)ethoxy)ethyl methacrylate) (PEG45-b-P(DPA55-co-PgTEGMA4)) and poly(l-histidine) (PHis). PEG45-b-P(DPA55-co-PgTEGMA4) was synthesized by atom transfer radical polymerization (ATRP), and was coinfiltrated with PHis into poly(methacrylic acid) (PMA)-coated MS particles assembled from different peptide-to-polymer ratios (1:1, 1:5, 1:10, or 1:15). Subsequent removal of the sacrificial templates and PMA resulted in monodisperse, colloidally stable, noncovalently cross-linked polymer-peptide blend replica particles that were stabilized by a combination of hydrophobic interactions between the PDPA and the PHis, hydrogen bonding between the PEG and PHis backbone, and π-π stacking of the imidazole rings of PHis side chains at physiological pH (pH ∼ 7.4). The synergistic charge-switchable properties of PDPA and PHis, and the enzymatic degradability of PHis, make these particles responsive to pH and enzymes. In vitro studies, in simulated endosomal conditions and inside cells, demonstrated that particle degradation kinetics could be engineered (from 2 to 8 h inside dendritic cells) based on simple adjustment of the peptide-to-polymer ratio used.
Publisher: American Chemical Society (ACS)
Date: 19-09-2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1NR08229A
Abstract: Mung bean-derived nanoparticles exhibit antioxidant activity to reduce reactive oxygen species, which can modulate the immune microenvironment and effectively inhibit psoriasiform skin inflammation.
Publisher: Royal Society of Chemistry (RSC)
Date: 2012
DOI: 10.1039/C2JM33737A
Publisher: American Chemical Society (ACS)
Date: 25-09-2023
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CC01874H
Abstract: Confined sono-polymerization is developed to prepare poly(ethylene glycol) nanoparticles within water-in-oil microemulsions for targeted delivery.
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C1SM05635B
Publisher: Wiley
Date: 09-02-2022
Abstract: The rapid and facile synthesis of hot melt super glue (HMSG) via the formation of adhesive supramolecular networks between catechol or pyrogallol hydroxyl groups (−OH) of polyphenols and repeat units (−CH 2 CH 2 O−) of poly(ethylene glycol) (PEG) based on hydrogen bonds is reported. The adhesion strength of HMSG, processed by heating–cooling of polyphenols and PEG without additional solvents, can be tuned up to 8.8 MPa via changing the molecular weight of PEG and the ratio of hydrogen bonding donors and receptors. The advantages of the reported HMSG lie in the ease and scalability of the assembly process, rapid adhesion on various substrates with excellent processability, resistance of low temperature and organic solvents, and recyclable adhesion strength. The solvent‐free HMSG represents a promising adhesive supramolecular network to expand the versatility and application of polyphenol‐based materials.
Publisher: American Chemical Society (ACS)
Date: 23-01-2020
Abstract: Injectable and sprayable hydrogels have attracted considerable attention for application in the biomedical field owing to their high moldability and efficiency in encapsulating therapeutics and cells. Herein, we report the spontaneous assembly of injectable and sprayable hydrogels via a one-step mixing of solutions of tannic acid (TA) and
Publisher: Elsevier BV
Date: 12-2022
Publisher: American Chemical Society (ACS)
Date: 13-12-2020
Abstract: We report the assembly of dual-responsive polypeptide nanoparticles loaded with indocyanine green (ICG) using a mesoporous silica (MS) templating method for photothermal and photodynamic therapy. Polypeptide nanoparticles composed of thiol-modified polylysine (PLL) are cross-linked with disulfide bonds and modified with poly(ethylene glycol) (PEG) and pH-sheddable dimethylmaleic anhydride (DMMA), which exhibit reduction- and pH-responsiveness. Cross-linking with disulfide bonds does not influence the free amine groups on PLL chains for further cargo conjugation and surface modification. The stripped DMMA at acidic pH reverses the zeta potential of PLL nanoparticles from negative to positive charge and subsequently results in high cell association. The thermo-responsiveness and singlet oxygen generation of the loaded ICG in DMMA-modified PLL nanoparticles are comparable to those of free ICG under laser irradiation, which induces higher cytotoxicity to cancer cells compared to succinic anhydride (SA)-modified PLL nanoparticles that are not pH-responsive. The reported dual-responsive PLL nanoparticles provide a promising platform for improved photothermal and photodynamic therapy.
Publisher: Wiley
Date: 10-07-2014
Abstract: The engineering of layer-by-layer (LbL) hybrid click capsules that are responsive to biological stimuli is reported. The capsules comprise a pH-sheddable, non cross-linked outer coating that protects enzyme-cleavable inner layers. Upon cellular uptake, the outer coating is released and the capsules are enzymatically degraded. In vitro cell degradation results in rapid capsule degradation (10 min) upon cellular internalization.
Publisher: American Chemical Society (ACS)
Date: 28-10-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0TB00405G
Abstract: Theranostic nanoparticles composed of hiphilic paramagnetic polymers are assembled for dual mode imaging and synergistic therapy.
Publisher: Wiley
Date: 27-12-2014
Abstract: A novel class of nanoparticles is developed for the co-delivery of a short cell penetrating peptide and a chemotherapeutic drug to achieve enhanced cytotoxicity. Tunable cytotoxicity is achieved through non-toxic peptide-facilitated gating. The strategy relies on a one-step blending process from polymer building blocks to form monodisperse, PEGylated particles that are sensitive to cellular pH variations. By varying the amount of peptide loading, the chemotherapeutic effects can be enhanced by up to 30-fold.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1CC02233D
Abstract: An activity-based Cu 2+ fluorescent probe functions through chelation with Cu 2+ via dye-based multidentate binding, which in turn specifically triggers the probe to undergo hydrolysis to release a NIR emission with AIE + ESIPT properties.
Publisher: American Chemical Society (ACS)
Date: 13-09-2021
Publisher: American Chemical Society (ACS)
Date: 22-03-2021
Publisher: American Chemical Society (ACS)
Date: 07-06-2018
Publisher: Elsevier BV
Date: 02-2019
DOI: 10.1016/J.JCIS.2018.10.037
Abstract: Covalent grafting and electrostatic-driven assembly have been two strategies in constructing well-defined polyoxometalate (POM) assemblies to produce specific morphologies and desirable properties. The modification of anionic counter-ions of hiphilic compounds in POM-surfactant hybrid systems is still unexploited. Herein, we report the co-assembly of a synthetic double-tailed magnetic surfactant (MagSurf), (C
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1BM00866H
Abstract: A potent ionizable lipid for in vitro and in vivo mRNA delivery was identified through the optimization of lipid amine-head groups.
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D2TA07834A
Abstract: Stretchable and tough double-network hydrogels mediated by CaCO 3 microparticles can be used to monitor human motions and mild pain signals at the wound site.
Publisher: Wiley
Date: 12-11-2011
Abstract: Inverse opal films with unique optical properties have potential as photonic crystal materials and have stimulated wide interest in recent years. Herein, iridescent hybrid polystyrene/nanoparticle macroporous films have been prepared by using the breath-figure method. The honeycomb-patterned thin films were prepared by casting gold nanoparticle-doped polystyrene solutions in chloroform at high relative humidity. Highly ordered hexagonal arrays of monodisperse pores with an average diameter of 880 nm are obtained. To account for the observed features, a microscopic phase separation of gold nanoparticles is proposed to occur in the breath-figure formation. That is, in idual gold nanoparticles adsorb at the solution/water interface and effectively stabilize condensed water droplets on the solution surface in a hexagonal array. Alternatively, at high nanoparticle concentrations the combination of breath-figure formation and nanoparticle phase separation leads to hierarchical structures with spherical aggregates under a honeycomb monolayer. The films show large features in both the visible and NIR regions that are attributed to a combination of nanoparticle and ordered-array absorptions. Organic ligand-stabilized CdSe/CdS quantum dots or Fe(3)O(4) nanoparticles may be loaded into the honeycomb structure to further modify the films. These results demonstrate new methods for the fabrication and functionalization of inverse opal films with potential applications in photonic and microelectronic materials.
Publisher: American Chemical Society (ACS)
Date: 16-10-2014
DOI: 10.1021/BM501171J
Abstract: This paper reports a facile and robust mold-templated technique for the assembly of mesoporous silica (MS) supraparticles and demonstrates their potential as vehicles for codelivery of brain-derived neurotrophic factor (BDNF) and dexamethasone (DEX). The MS supraparticles are assembled using gelatin as a biodegradable adhesive to bind and cross-link the particles. Microfabricated molds made of polydimethylsiloxane are used to control the size and shape of the supraparticles. The obtained mesoporous silica-gelatin hybrid supraparticles (MSG-SPs) are stable in water as well as in organic solvents, such as dimethyl sulfoxide, and efficiently coencapsulate both BDNF and DEX. The MSG-SPs also exhibit sustained release kinetics in simulated physiological conditions (>30 days), making them potential candidates for long-term delivery of therapeutics to the inner ear.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1PY00947H
Abstract: The anticancer drug of Bortezomib conjugated onto catechol-modified bottlebrush block copolymers can be intracellularly released owing to the pH-responsive behavior, resulting in considerable cell death and tumor growth inhibition.
Publisher: American Chemical Society (ACS)
Date: 13-01-2021
Publisher: American Chemical Society (ACS)
Date: 16-06-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4CC08759C
Abstract: Surface-confined ultra-thin polyrotaxane (PRX)-based films with tunable composition, surface topology and swelling characteristics were prepared by solid-state continuous assembly of polymers (ssCAP).
Publisher: American Association for the Advancement of Science (AAAS)
Date: 12-07-2013
Abstract: Thin adherent films formed from ferric ions and a natural polyphenol, tannic acid, can coat a wide variety of surfaces. [Also see Perspective by Bentley and Payne ]
Publisher: Springer Science and Business Media LLC
Date: 10-10-2016
Abstract: The organized assembly of particles into superstructures is typically governed by specific molecular interactions or external directing factors associated with the particle building blocks, both of which are particle-dependent. These superstructures are of interest to a variety of fields because of their distinct mechanical, electronic, magnetic and optical properties. Here, we establish a facile route to a erse range of superstructures based on the polyphenol surface-functionalization of micro- and nanoparticles, nanowires, nanosheets, nanocubes and even cells. This strategy can be used to access a large number of modularly assembled superstructures, including core-satellite, hollow and hierarchically organized supraparticles. Colloidal-probe atomic force microscopy and molecular dynamics simulations provide detailed insights into the role of surface functionalization and how this facilitates superstructure construction. Our work provides a platform for the rapid generation of superstructured assemblies across a wide range of length scales, from nanometres to centimetres.
Publisher: American Chemical Society (ACS)
Date: 26-05-2022
DOI: 10.1021/ACS.LANGMUIR.2C01117
Abstract: Tuning the physicochemical parameters (e.g., size, shape, and surface chemistry) of colloidal particles (CPs) for the engineering of drug carriers has proven to be a promising approach to improve drug delivery efficacy. Recently, the stiffness of CPs has attracted widespread attention for modulating bio-nano interactions. In this perspective, we outline the strategies for the modulation and characterization of CP stiffness and highlight the importance of CP stiffness in the control over biological interactions. Challenges and opportunities of current and future developments in the modulation of CP stiffness for the exploration of bio-nano interactions in therapeutic delivery are also discussed. This perspective is expected to help thoroughly understand the role of CP stiffness in bio-nano interactions and facilitate the design of CPs as carriers for improved drug and vaccine delivery.
Publisher: American Chemical Society (ACS)
Date: 13-03-2017
DOI: 10.1021/JACS.6B11302
Abstract: Peptides perform a erse range of physiologically important functions. The formulation of nanoparticles directly from functional peptides would therefore offer a versatile and robust platform to produce highly functional therapeutics. Herein, we engineered proapoptotic peptide nanoparticles from mitochondria-disrupting KLAK peptides using a template-assisted approach. The nanoparticles were designed to disassemble into free native peptides via the traceless cleavage of disulfide-based cross-linkers. Furthermore, the cytotoxicity of the nanoparticles was tuned by controlling the kinetics of disulfide bond cleavage, and the rate of regeneration of the native peptide from the precursor species. In addition, a small molecule drug (i.e., doxorubicin hydrochloride) was loaded into the nanoparticles to confer synergistic cytotoxic activity, further highlighting the potential application of KLAK particles in therapeutic delivery.
Publisher: American Chemical Society (ACS)
Date: 25-09-2017
Abstract: Surface modification is frequently used to tailor the interactions of nanoparticles with biological systems. In many cases, the chemical nature of the treatments employed to modify the biological interface (for ex le attachment of hydrophilic polymers or targeting groups) is the focus of attention. However, isolation of the fundamental effects of the materials employed to modify the interface are often confounded by secondary effects imparted by the underlying substrate. Herein, we demonstrate that polymer replica particles templated from degradable mesoporous silica provide a facile means to evaluate the impact of surface modification on the biological interactions of nanomaterials, independent of the substrate. Poly(ethylene glycol) (PEG), poly(N-(2 hydroxypropyl)methacrylamide) (PHPMA), and poly(methacrylic acid) (PMA) were templated onto mesoporous silica and cross-linked and the residual particles were removed. The resulting nanoparticles, comprising interfacial polymer alone, were then investigated using a range of in vitro and in vivo tests. As expected, the PEG particles showed the best stealth properties, and these trends were consistent in both in vitro and in vivo studies. PMA particles showed the highest cell association in cell lines in vitro and were rapidly taken up by monocytes in ex vivo whole blood, properties consistent with the very high in vivo clearance subsequently seen in rats. In contrast, PHPMA particles showed rapid association with both granulocytes and monocytes in ex vivo whole blood, even though in vivo clearance was less rapid than the PMA particles. Rat studies confirmed better systemic exposure for PEG and PHPMA particles when compared to PMA particles. This study provides a new avenue for investigating material-dependent biological behaviors of polymer particles, irrespective of the properties of the underlying core, and provides insights for the selection of polymer particles for future biological applications.
Publisher: American Chemical Society (ACS)
Date: 21-01-2015
DOI: 10.1021/NN5061578
Abstract: We report the engineering of poly(ethylene glycol) (PEG) hydrogel particles using a mesoporous silica (MS) templating method via tuning the PEG molecular weight, particle size, and the presence or absence of the template and investigate the cell association and biodistribution of these particles. An ex vivo assay based on human whole blood that is more sensitive and relevant than traditional cell-line based assays for predicting in vivo circulation behavior is introduced. The association of MS@PEG particles (template present) with granulocytes and monocytes is higher compared with PEG particles (template absent). Increasing the PEG molecular weight (from 10 to 40 kDa) or decreasing the PEG particle size (from 1400 to 150 nm) reduces phagocytic blood cell association of the PEG particles. Mice biodistribution studies show that the PEG particles exhibit extended circulation times (>12 h) compared with the MS@PEG particles and that the retention of smaller PEG particles (150 nm) in blood, when compared with larger PEG particles (>400 nm), is increased at least 4-fold at 12 h after injection. Our findings highlight the influence of unique aspects of polymer hydrogel particles on biological interactions. The reported PEG hydrogel particles represent a new class of polymer carriers with potential biomedical applications.
Publisher: Elsevier BV
Date: 04-2021
Publisher: Wiley
Date: 09-2015
Abstract: Nanoporous metal-phenolic particles are fabricated through the nanostructural replication of dense Fe
Publisher: American Chemical Society (ACS)
Date: 28-04-2020
Publisher: No publisher found
Date: 2010
Publisher: Elsevier BV
Date: 09-2018
Publisher: American Chemical Society (ACS)
Date: 22-08-2018
DOI: 10.1021/ACS.LANGMUIR.8B02117
Abstract: The assembly of particles composed solely or mainly of poly(ethylene glycol) (PEG) is an emerging area that is gaining increasing interest within bio-nano science. PEG, widely considered to be the "gold standard" among polymers for drug delivery, is providing a platform for exploring fundamental questions and phenomena at the interface between particle engineering and biomedicine. These include the targeting and stealth behaviors of synthetic nanomaterials in biological environments. In this feature article, we discuss recent work in the nanoengineering of PEG particles and explore how they are enabling improved targeting and stealth performance. Specific ex les include PEG particles prepared through surface-initiated polymerization, mesoporous silica replication via postinfiltration, and particle assembly through metal-phenolic coordination. This particle class exhibits unique in vivo behavior (e.g., biodistribution and immune cell interactions) and has recently been explored for drug delivery applications.
Publisher: Wiley
Date: 27-12-2014
Abstract: The synthesis of cross-linker free layer-by-layer (LbL) capsules that solely utilize cellular pH variations as a trigger to specifically deconstruct and subsequently release cargo in cells is reported. These capsules demonstrate retention of water-soluble therapeutic molecules as small as 500 Da at extracellular pH. Triggered capsule degradation and release of cargo is observed within 30 min of cell uptake.
Publisher: American Chemical Society (ACS)
Date: 24-05-2021
Publisher: American Chemical Society (ACS)
Date: 12-08-2014
DOI: 10.1021/LA502176G
Abstract: Polymer microcapsules can be used as bioreactors and artificial cells however, preparation methods for cell-like microcapsules are typically time-consuming, low yielding, and/or involve custom microfluidics. Here, we introduce a rapid (∼30 min per batch, eight layers), scalable (up to 500 mg of templates), and efficient (98% yield) microcapsule preparation technique utilizing a fluidized bed for the layer-by-layer (LbL) assembly of polymers, and we investigate the parameters that govern the formation of robust capsules. Fluidization in water was possible for particles of comparable diameter to mammalian cells (>5 μm), with the experimental flow rates necessary for fluidization matching well with the theoretical values. Important variables for polymer film deposition and capsule formation were the concentration of polymer solution and the molecular weight of the polymer, while the volume of the polymer solution had a negligible impact. In combination, increasing the polymer molecular weight and polymer solution concentration resulted in improved film deposition and the formation of robust microcapsules. The resultant polymer microcapsules had a thickness of ∼5.5 nm per bilayer, which is in close agreement with conventionally prepared (quiescent (nonflow) adsorption/centrifugation/wash) LbL capsules. The technique reported herein provides a new way to rapidly generate microcapsules (approximately 8 times quicker than the conventional means), while being also amenable to scale-up and mass production.
Publisher: Wiley
Date: 20-02-2023
Abstract: Nanostructured materials with tunable structures and functionality are of interest in erse areas. Herein, metal ions are coordinated with quinones through metal‐acetylacetone coordination bonds to generate a class of structurally tunable, universally adhesive, hydrophilic, and pH‐degradable materials. A library of metal‐quinone networks (MQNs) is produced from five model quinone ligands paired with nine metal ions, leading to the assembly of particles, tubes, capsules, and films. Importantly, MQNs show bidirectional pH‐responsive disassembly in acidic and alkaline solutions, where the quinone ligands mediate the disassembly kinetics, enabling temporal and spatial control over the release of multiple components using multilayered MQNs. Leveraging this tunable release and the inherent medicinal properties of quinones, MQN prodrugs with a high drug loading ( wt %) are engineered using doxorubicin for anti‐cancer therapy and shikonin for the inhibition of the main protease in the SARS‐CoV‐2 virus.
Publisher: American Chemical Society (ACS)
Date: 04-07-2023
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0CC01727B
Abstract: We report thermo-responsive gels of polyacrylamide (PAAm) with ionic surfactants in mixed water and ethylene glycol (W–EG) solvents as smart windows to solubilize ultraviolet absorbents for UV shielding materials.
Publisher: American Chemical Society (ACS)
Date: 13-04-2020
Publisher: American Chemical Society (ACS)
Date: 09-10-2020
DOI: 10.1021/ACSMACROLETT.0C00557
Abstract: Poly(ethylene glycol) (PEG) is the most used hydrophilic polymer for low-fouling coatings to minimize nonspecific interactions. The PEG molecular weight or its length as well as surface density are typically considered as the main impacts on the control over low-fouling properties. However, the influence of PEG monodispersity on such investigations is typically ignored and rarely reported. Herein, we report the assembly of PEGylated coatings on planar surfaces and Au nanorods (AuNRs) using a series of monodisperse PEG (Mono-PEG) with exact molecular weights and commonly used polydisperse PEG (Poly-PEG) to investigate the effect of the PEG molecular weight and monodispersity on the low-fouling properties. Nonspecific interactions with proteins or cells on PEGylated planar surfaces can be significantly reduced when Mono-PEG with a molecular weight of 752 Da and above is used, while a higher average molecular weight of 2000 Da is required for Poly-PEG-modified surfaces. Cell association of PEGylated AuNRs further confirms that a low molecular weight of Mono-PEG is sufficient to achieve low-fouling properties. This study provides an insight and general guidance into the engineering of low-fouling surfaces by the appropriate choice based on the PEG monodispersity and/or molecular weights.
Publisher: American Chemical Society (ACS)
Date: 16-05-2014
DOI: 10.1021/LA501324R
Abstract: We report a templating approach for the preparation of functional polymer replica particles via surface-initiated polymerization in mesoporous silica templates. Subsequent removal of the template resulted in discrete polymer particles. Furthermore, redox-responsive replica particles could be engineered to disassemble in a reducing environment. Particles, made of poly(methacryloyloxyethyl phosphorylcholine) (PMPC) or poly[oligo(ethylene glycol) methyl ether methacrylate] (POEGMA), exhibited very low association to human cancer cells (below 5%), which renders the reported charge-neutral polymer particles a modular and versatile class of highly functional carriers with potential applications in drug delivery.
Publisher: American Chemical Society (ACS)
Date: 05-09-2012
DOI: 10.1021/NN302024T
Abstract: We report the sequential assembly of proteins via the alternating physical adsorption of human serum albumin (HSA) and chemical grafting with isobutyramide (IBAM) or bromoisobutyramide (BrIBAM) groups. This approach, performed on silica template particles, leads to the formation of noncovalent protein films with controlled growth at the nanometer scale. Further, after template removal, hollow protein capsules with tunable wall thicknesses and high mechanical stability are obtained. The use of BrIBAM, compared to IBAM grafts, leads to significantly thicker capsule walls, highlighting the influence of the bromine atoms in the assembly process, which is discussed in terms of a theoretical model of noncovalent interactions. Another feature of the process is the possibility to functionalize the HSA capsules with other biologically active macromolecules, including enzymes, polysaccharides, or DNA plasmids, demonstrating the versatility of this approach. We also report that BrIBAM-HSA and IBAM-HSA capsules display negligible cytotoxicity in vitro with HeLa cells and that their cellular uptake is dependent on the thickness of the capsule walls. These findings support the potential use of these protein capsules in tailored biological applications such as drug delivery.
Publisher: Wiley
Date: 14-03-2019
Abstract: Low-fouling or "stealth" particles composed of poly(ethylene glycol) (PEG) display a striking ability to evade phagocytic cell uptake. However, functionalizing them for specific targeting is challenging. To address this challenge, stealth PEG particles prepared by a mesoporous silica templating method are functionalized with bispecific antibodies (BsAbs) to obtain PEG-BsAb particles via a one-step binding strategy for cell and tumor targeting. The dual specificity of the BsAbs-one arm binds to the PEG particles while the other targets a cell antigen (epidermal growth factor receptor, EGFR)-is exploited to modulate the number of targeting ligands per particle. Increasing the BsAb incubation concentration increases the amount of BsAb tethered to the PEG particles and enhances targeting and internalization into breast cancer cells overexpressing EGFR. The degree of BsAb functionalization does not significantly reduce the stealth properties of the PEG particles ex vivo, as assessed by their interactions with primary human blood granulocytes and monocytes. Although increasing the BsAb amount on PEG particles does not lead to the expected improvement in tumor accumulation in vivo, BsAb functionalization facilitates tumor cell uptake of PEG particles. This work highlights strategies to balance evading nonspecific clearance pathways, while improving tumor targeting and accumulation.
Publisher: American Chemical Society (ACS)
Date: 05-02-2015
DOI: 10.1021/BM5017139
Abstract: Metal-phenolic coordination chemistry provides a simple and rapid way to fabricate ultrathin films. Here, we report a facile strategy for the preparation of low-fouling and pH-degradable metal-phenolic network (MPN) capsules using a synthetic polyphenol derivative, poly(ethylene glycol) (PEG)-polyphenol, as a building block. PEG-MPN capsules exhibit reduced nonspecific protein adsorption and cell association compared with tannic acid (TA)-MPN capsules. In addition, they show faster disassembly at a biologically relevant pH (5) than TA-MPN capsules (80% in 5 h vs 30% in 10 days). PEG-MPN capsules combine both the low fouling properties of PEG and the advantages of the MPN-driven assembly process (e.g., fast assembly and pH-degradability).
Publisher: Wiley
Date: 02-09-2022
Abstract: Cation–π interaction is one of the most important noncovalent interactions found in biosystems, which has attracted great interests for the engineering of functional materials. In this work, one‐step assembly of super‐hydrophilic coatings via surface modification with polyphenols and cations is reported based on cation–π interactions. Hydrophilicity of surface coatings is tunable by the variation of cations based on the different affinity between polyphenols and cations. Copper meshes coated with tannic acid and tetramethylammonium demonstrate super‐hydrophilicity and high stability due to the strong cation–π interaction between catechol yrogallol and cations. The super‐hydrophilic coatings show high oil breakthrough pressure, self‐cleaning, and anti‐fogging properties, which can efficiently separate the mixture of oil and water. This study provides an avenue to explore the cation–π interactions for super‐hydrophilic coatings.
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C4NR02623C
Abstract: We report the preparation of albumin-based nanoparticles assembled via isobutyramide groups providing simultaneous magnetic resonance imaging and cellular gene silencing.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1QM00295C
Abstract: The use of biologically-derived nanoparticles from mung beans for combination chemo-ferroptosis therapy and magnetic resonance imaging is reported, which highlights the potential of the nanoparticles for biomedical applications.
Publisher: Elsevier BV
Date: 12-2020
Publisher: Wiley
Date: 20-02-2023
Abstract: Nanostructured materials with tunable structures and functionality are of interest in erse areas. Herein, metal ions are coordinated with quinones through metal‐acetylacetone coordination bonds to generate a class of structurally tunable, universally adhesive, hydrophilic, and pH‐degradable materials. A library of metal‐quinone networks (MQNs) is produced from five model quinone ligands paired with nine metal ions, leading to the assembly of particles, tubes, capsules, and films. Importantly, MQNs show bidirectional pH‐responsive disassembly in acidic and alkaline solutions, where the quinone ligands mediate the disassembly kinetics, enabling temporal and spatial control over the release of multiple components using multilayered MQNs. Leveraging this tunable release and the inherent medicinal properties of quinones, MQN prodrugs with a high drug loading ( wt %) are engineered using doxorubicin for anti‐cancer therapy and shikonin for the inhibition of the main protease in the SARS‐CoV‐2 virus.
Publisher: American Chemical Society (ACS)
Date: 13-01-2015
DOI: 10.1021/MZ5007443
Publisher: American Chemical Society (ACS)
Date: 17-06-2011
DOI: 10.1021/CM201390E
Publisher: Wiley
Date: 16-05-2017
Abstract: Therapeutic nanoparticles hold clinical promise for cancer treatment by avoiding limitations of conventional pharmaceuticals. Herein, a facile and rapid method is introduced to assemble poly(ethylene glycol) (PEG)-modified Pt prodrug nanocomplexes through metal-polyphenol complexation and combined with emulsification, which results in ≈100 nm diameter nanoparticles (PtP NPs) that exhibit high drug loading (0.15 fg Pt per nanoparticle) and low fouling properties. The PtP NPs are characterized for potential use as cancer therapeutics. Mass cytometry is used to quantify uptake of the nanoparticles and the drug concentration in in idual cells in vitro. The PtP NPs have long circulation times, with an elimination half-life of ≈18 h in healthy mice. The in vivo antitumor activity of the PtP NPs is systematically investigated in a human prostate cancer xenograft mouse model. Mice treated with the PtP NPs demonstrate four times better inhibition of tumor growth than either free prodrug or cisplatin. This study presents a promising strategy to prepare therapeutic nanoparticles for biomedical applications.
Publisher: American Chemical Society (ACS)
Date: 13-07-2012
DOI: 10.1021/BM300835R
Abstract: We report a facile approach to immobilize pH-cleavable polymer-drug conjugates in mussel-inspired polydopamine (PDA) capsules for intracellular drug delivery. Our design takes advantage of the facile PDA coating to form capsules, the chemical reactivity of PDA films, and the acid-labile groups in polymer side chains for sustained pH-induced drug release. The anticancer drug doxorubicin (Dox) was conjugated to thiolated poly(methacrylic acid) (PMA(SH)) with a pH-cleavable hydrazone bond, and then immobilized in PDA capsules via robust thiol-catechol reactions between the polymer-drug conjugate and capsule walls. The loaded Dox showed limited release at physiological pH but significant release (over 85%) at endosomal/lysosomal pH. Cell viability assays showed that Dox-loaded PDA capsules enhanced the efficacy of eradicating HeLa cancer cells compared with free drug under the same assay conditions. The reported method provides a new platform for the application of stimuli-responsive PDA capsules as drug delivery systems.
Publisher: American Chemical Society (ACS)
Date: 17-03-2017
DOI: 10.1021/ACS.LANGMUIR.6B04591
Abstract: It is difficult to synthesize magnetic gold nanoparticles (AuNPs) with ultrafine sizes (<2 nm) based on a conventional method via coating AuNPs using magnetic particles, compounds, or ions. Here, magnetic cationic surfactants C
Publisher: Wiley
Date: 10-09-2014
Abstract: Super-soft PEG hydrogel particles with tunable elasticity are prepared via a mesoporous silica templating method. The deformability behavior of these particles, in a microfluidic blood-capillary model, can be tailored to be similar to that of human red blood cells. These results provide a new platform for the design and development of soft hydrogel particles for investigating bio-nano interactions.
Publisher: Wiley
Date: 18-06-2015
Abstract: Dual-responsive boronate-phenolic network (BPN) capsules are fabricated by the complexation of phenylborate and phenolic materials. The BPN capsules are stable in the presence of competing carbohydrates, but dissociate at acidic pH or in the presence of competing cis-diols at physiological pH. This engineered capsule system provides a platform for a wide range of biological and biomedical applications.
Publisher: American Chemical Society (ACS)
Date: 28-05-2013
DOI: 10.1021/NN401800U
Abstract: Nanoporous polymer particles (NPPs) prepared by mesoporous silica templating show promise as a new class of versatile drug/gene delivery vehicles owning to their high payload capacity, functionality, and responsiveness. Understanding the cellular dynamics of such particles, including uptake, intracellular trafficking, and distribution, is an important requirement for their development as therapeutic carriers. Herein, we examine the spatiotemporal map of the cellular processing of submicrometer-sized disulfide-bonded poly(methacrylic acid) (PMASH) NPPs in HeLa cells using both flow cytometry and fluorescence microscopy. The data show that the PMASH NPPs are transported from the early endosomes to the lysosomes within a few minutes. Upon cell ision, the lysosome-enclosed PMASH NPPs are distributed asymmetrically between two daughter cells. Statistical analysis of cells during cytokinesis suggests that partitioning of particles is biased with an average segregation deviation of 60%. Further, two-dimensional difference gel electrophoresis (2D-DIGE) analysis reveals that 127 out of 3059 identified spots are differentially regulated upon exposure to the PMASH NPPs. Pathway analysis of the proteomics data suggests that ubiquitylation, a reversible modification of cellular proteins with ubiquitin, plays a central role in overall cellular responses to the particles. These results provide important insights into the cellular dynamics and heterogeneity of NPPs, as well as the mechanisms that regulate the motility of these particles within cells, all of which have important implications for drug susceptibility characteristics in cancer cells using particle-based carriers.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1CC06943H
Abstract: Nanoparticles for immuno-photothermal therapy were constructed by encapsulating photosensitizers and aluminum ions into zeolitic imidazolate framework-8, which significantly inhibited the growth of primary and rechallenged tumors.
Publisher: Wiley
Date: 03-08-2015
Abstract: Smart poly(2-oxazoline) (POx)-based multifunctional polymer capsules that specifically target glycoprotein (GP) IIb/IIIa on the surface of activated platelets are degraded by the serine protease thrombin and release the urokinase plasminogen activator loaded into the polymer capsules, only in the area of acute thrombosis.
Publisher: American Chemical Society (ACS)
Date: 25-07-2013
DOI: 10.1021/LA402146T
Abstract: Soft hydrogel particles with tunable mechanical properties are promising for next-generation therapeutic applications. This is due to the increasingly proven role that physicochemical properties play in particulate-based delivery vectors, both in vitro and in vivo. The ability to understand and quantify the mechanical properties of such systems is therefore essential to optimize function and performance. We report control over the mechanical properties of poly(methacrylic acid) (PMA) hydrogel particles based on a mesoporous silica templating method. The mechanical properties of the obtained particles can be finely tuned through variation of the cross-linker concentration, which is hereby quantified using a cross-linking polymer with a fluorescent tag. We demonstrate that the mechanical properties of the particles can be elucidated using an atomic force microscopy (AFM) force spectroscopy method, which additionally allows for the study of hydrogel material properties at the nanoscale through high-resolution force mapping. Young's modulus and stiffness of the particles were tuned between 0.04 and 2.53 MPa and between 1.6 and 28.4 mN m(-1), respectively, through control over the cross-linker concentration. The relationship between the concentration of the cross-linker added and the amount of adsorbed polymer was observed to follow a Langmuir isotherm, and this relationship was found to correlate linearly with the particle mechanical properties.
Publisher: Elsevier BV
Date: 05-2014
DOI: 10.1016/J.CIS.2013.10.012
Abstract: Hollow polymer capsules are attracting increasing research interest due to their potential application as drug delivery vectors, sensors, biomimetic nano- or multi-compartment reactors and catalysts. Thus, significant effort has been directed toward tuning their size, composition, morphology, and functionality to further their application. In this review, we provide an overview of emerging techniques for the fabrication of polymer capsules, encompassing: self-assembly, layer-by-layer assembly, single-step polymer adsorption, bio-inspired assembly, surface polymerization, and ultrasound assembly. These techniques can be applied to prepare polymer capsules with erse functionality and physicochemical properties, which may fulfill specific requirements in various areas. In addition, we critically evaluate the challenges associated with the application of polymer capsules in drug delivery systems.
Publisher: Elsevier BV
Date: 05-2008
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1BM01139A
Abstract: Self-assembled nanoparticles composed of photosensitizers and immune adjuvants are reported for combination photodynamic immunotherapy to inhibit both primary and distant tumors.
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C3SM53056F
Abstract: We report a versatile approach for the design of substrate-independent low-fouling surfaces via mussel-inspired immobilisation of zwitterionic peptides. Using mussel-inspired polydopamine (PDA) coatings, zwitterionic glutamic acid- and lysine-based peptides were immobilised on various substrates, including noble metals, metal oxides, polymers, and semiconductors. The variation of surface chemistry and surface wettability upon surface treatment was monitored with X-ray photoelectron spectroscopy (XPS) and water contact angle measurements. Following peptide immobilisation, the surfaces became more hydrophilic due to the strong surface hydration compared with PDA-coated surfaces. The peptide-functionalised surfaces showed resistance to human blood serum adsorption and also effectively prevented the adhesion of gram-negative and gram-positive bacteria (i.e., Escherichia coli and Staphylococcus epidermidis) and mammalian cells (i.e., NIH 3T3 mouse embryonic fibroblast cells). The versatility of mussel-inspired chemistry combined with the unique biological nature and tunability of peptides allows for the design of low-fouling surfaces, making this a promising coating technique for various applications.
Publisher: Elsevier BV
Date: 02-2020
Publisher: Wiley
Date: 25-05-2010
Publisher: Wiley
Date: 07-10-2013
Abstract: We report a versatile approach for polymer capsule preparation using immobilized particles, which are immersed into polymer solutions either manually or by using an automated robotic dipping machine. This technique produces polyelectrolyte capsules with improved retention over conventionally prepared capsules. Additionally, responsive hydrogel capsules of different diameter can be prepared simultaneously.
Publisher: Wiley
Date: 09-05-2013
Publisher: American Chemical Society (ACS)
Date: 30-10-2015
Publisher: Elsevier BV
Date: 04-2019
DOI: 10.1016/J.CIS.2019.01.005
Abstract: Microgels are colloidal particles with crosslinked polymer networks and dimensions ranging from tens of nanometers to micrometers. Specifically, smart microgels are fascinating capable of responding to biological signals in vivo or remote triggers and making the possible for applications in biomaterials and biomedicines. Therefore, how to fundamentally design microgels is an urgent problem to be solved. In this review, we put forward our important fundamental opinions on how to devise the intelligent microgels for cancer therapy, biosensing and biological lubrication. We focus on the design ideas instead of specific implementation process by employing reverse synthesis analysis to programme the microgels at the original stage. Moreover, special insights will be, for the first time, as far as we know, dedicated to the particles completely composed of DNA or proteins into microgel systems. These are discussed in detail in this review. We expect to give readers a broad overview of the design criteria and practical methodologies of microgels according to the application fields, as well as to propel the further developments of highly interesting concepts and materials.
Publisher: No publisher found
Date: 2010
Publisher: American Chemical Society (ACS)
Date: 26-08-2019
DOI: 10.1021/ACS.BIOMAC.9B00925
Abstract: Drug carriers typically require both stealth and targeting properties to minimize nonspecific interactions with healthy cells and increase specific interaction with diseased cells. Herein, the assembly of targeted poly(ethylene glycol) (PEG) particles functionalized with cyclic peptides containing Arg-Gly-Asp (RGD) (ligand) using a mesoporous silica templating method is reported. The influence of PEG molecular weight, ligand-to-PEG molecule ratio, and particle size on cancer cell targeting to balance stealth and targeting of the engineered PEG particles is investigated. RGD-functionalized PEG particles (PEG-RGD particles) efficiently target U-87 MG cancer cells under static and flow conditions in vitro, whereas PEG and cyclic peptides containing Arg-Asp-Gly (RDG)-functionalized PEG (PEG-RDG) particles display negligible interaction with the same cells. Increasing the ligand-to-PEG molecule ratio improves cell targeting. In addition, the targeted PEG-RGD particles improve cell uptake via receptor-mediated endocytosis, which is desirable for intracellular drug delivery. The PEG-RGD particles show improved tumor targeting (14% ID g
Publisher: American Chemical Society (ACS)
Date: 04-09-2020
Publisher: American Chemical Society (ACS)
Date: 10-05-2022
DOI: 10.1021/ACS.CHEMREV.1C01042
Abstract: Metal ions are ubiquitous in nature and play significant roles in assembling functional materials in fields spanning chemistry, biology, and materials science. Metal-phenolic materials are assembled from phenolic components in the presence of metal ions through the formation of metal-organic complexes. Alkali, alkali-earth, transition, and noble metal ions as well as metalloids interacting with phenolic building blocks have been widely exploited to generate erse hybrid materials. Despite extensive studies on the synthesis of metal-phenolic materials, a comprehensive summary of how metal ions guide the assembly of phenolic compounds is lacking. A fundamental understanding of the roles of metal ions in metal-phenolic materials engineering will facilitate the assembly of materials with specific and functional properties. In this review, we focus on the ersity and function of metal ions in metal-phenolic material engineering and emerging applications. Specifically, we discuss the range of underlying interactions, including (i) cation-π, (ii) coordination, (iii) redox, and (iv) dynamic covalent interactions, and highlight the wide range of material properties resulting from these interactions. Applications (e.g., biological, catalytic, and environmental) and perspectives of metal-phenolic materials are also highlighted.
Publisher: American Chemical Society (ACS)
Date: 05-11-2020
Publisher: Wiley
Date: 18-06-2010
Publisher: Wiley
Date: 10-05-2013
Abstract: DNA-loaded polypeptide particles are prepared via templated assembly of mesoporous silica for the delivery of adjuvants. The elasticity and cargo-loading capacity of the obtained particles can be tuned by the amount of cross-linker used to stabilize the polypeptide particles. The use of polypeptide particles as biocarriers provides a promising method for vaccine delivery.
Publisher: American Chemical Society (ACS)
Date: 18-02-2009
DOI: 10.1021/JP808785J
Publisher: American Chemical Society (ACS)
Date: 28-03-2022
DOI: 10.1021/ACS.ACCOUNTS.2C00068
Abstract: Supramolecular assembly is commonly driven by noncovalent interactions (e.g., hydrogen bonding, electrostatic, hydrophobic, and aromatic interactions) and plays a predominant role in multidisciplinary research areas ranging from materials design to molecular biology. Understanding these noncovalent interactions at the molecular level is important for studying and designing supramolecular assemblies in chemical and biological systems. Cation-π interactions, initially found through their influence on protein structure, are generally formed between electron-rich π systems and cations (mainly alkali, alkaline-earth metals, and ammonium). Cation-π interactions play an essential role in many biological systems and processes, such as potassium channels, nicotinic acetylcholine receptors, biomolecular recognition and assembly, and the stabilization and function of biomacromolecular structures. Early fundamental studies on cation-π interactions primarily focused on computational calculations, protein crystal structures, and gas- and solid-phase experiments. With the more recent development of spectroscopic and nanomechanical techniques, cation-π interactions can be characterized directly in aqueous media, offering opportunities for the rational manipulation and incorporation of cation-π interactions into the design of supramolecular assemblies. In 2012, we reported the essential role of cation-π interactions in the strong underwater adhesion of Asian green mussel foot proteins deficient in l-3,4-dihydroxyphenylalanine (DOPA) via direct molecular force measurements. In another study in 2013, we reported the experimental quantification and nanomechanics of cation-π interactions of various cations and π electron systems in aqueous solutions using a surface forces apparatus (SFA).Over the past decade, much progress has been achieved in probing cation-π interactions in aqueous solutions, their impact on the underwater adhesion and cohesion of different soft materials, and the fabrication of functional materials driven by cation-π interactions, including surface coatings, complex coacervates, and hydrogels. These studies have demonstrated cation-π interactions as an important driving force for engineering functional materials. Nevertheless, compared to other noncovalent interactions, cation-π interactions are relatively less investigated and underappreciated in governing the structure and function of supramolecular assemblies. Therefore, it is imperative to provide a detailed overview of recent advances in understanding of cation-π interactions for supramolecular assembly, and how these interactions can be used to direct supramolecular assembly for various applications (e.g., underwater adhesion). In this Account, we present very recent advances in probing and applying cation-π interactions for mussel-inspired supramolecular assemblies as well as their structural and functional characteristics. Particular attention is paid to experimental characterization techniques for quantifying cation-π interactions in aqueous solutions. Moreover, the parameters responsible for modulating the strengths of cation-π interactions are discussed. This Account provides useful insights into the design and engineering of smart materials based on cation-π interactions.
Publisher: American Chemical Society (ACS)
Date: 29-06-2015
DOI: 10.1021/ACS.BIOMAC.5B00562
Abstract: We report the engineering of intracellular redox-responsive nanoporous poly(ethylene glycol)-poly(l-lysine) particles (NPEG-PLLs). The obtained particles exhibit no toxicity while maintaining the capability to deliver a small interfering RNA sequence (siRNA) targeting the anti-apoptotic factor, survivin, in prostate cancer cells. The redox-mediated cleavage of the disulfide bonds stabilizing the NPEG-PLL-siRNA complex results in the release of bioactive siRNA into the cytosol of prostate cancer PC-3 cells, which, in turn, leads to the effective silencing (∼59 ± 8%) of the target gene. These findings, obtained under optimal conditions, indicate that NPEG-PLLs may protect the therapeutic nucleic acid in the extracellular and intracellular environments, thus preventing the occurrence of competitive interactions with serum and cytosolic proteins as well as degradation by RNase. The intracellular trafficking and final fate of the NPEG-PLLs were investigated by a combination of deconvolution microscopy, fluorescence lifetime imaging microscopy, and super-resolution structured illumination microscopy. A significant impairment of cell survival was observed in cells concomitantly exposed to paclitaxel and siRNA-loaded NPEG-PLLs. Overall, our findings indicate that NPEG-PLLs represent a highly loaded depot for the delivery of therapeutic nucleic acids to cancer cells.
Publisher: CRC Press
Date: 17-12-2010
DOI: 10.1201/B10479-2
Publisher: CRC Press
Date: 17-12-2010
DOI: 10.1201/B10479-3
Publisher: American Chemical Society (ACS)
Date: 11-10-2023
Publisher: American Chemical Society (ACS)
Date: 07-10-2022
Abstract: Hepatitis B virus (HBV) infection remains a major challenge to global health due to unsatisfactory treatment efficacy, side effects of current therapies, and immune tolerance. Toll-like receptors 7/8 (TLR7/8) agonists have shown great potential in chronic hepatitis B (CHB) cure, but systemic administration often induces severe side effects due to rapid dispersion into the microvasculature. Herein, we encapsulate an imidazoquinoline-based TLR7/8 agonist (IMDQ) into zeolitic imidazolate framework 8 nanoparticles (IMDQ@ZIF-8 NPs) for HBV immunotherapy. Compared with free IMDQ, IMDQ@ZIF-8 NPs efficiently accumulate in the liver and are selectively taken up by antigen-presenting cells (APCs), leading to enhanced APC activation and efficient viral elimination in HBV-infected models. Strikingly, MDQ@ZIF-8 NP treatment results in the obvious production of anti-HBs antibody and seroconversion in HBV-infected mice. Overall, this study on the convergence of a facile assembly approach and efficient therapeutic effects represents a promising strategy for HBV treatment.
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3EN00471F
Publisher: American Chemical Society (ACS)
Date: 11-01-2017
Abstract: Despite the immense public health successes of immunization over the past century, effective vaccines are still lacking for globally important pathogens such as human immunodeficiency virus, malaria, and tuberculosis. Exciting recent advances in immunology and biotechnology over the past few decades have facilitated a shift from empirical to rational vaccine design, opening possibilities for improved vaccines. Some of the most important advancements include (i) the purification of subunit antigens with high safety profiles, (ii) the identification of innate pattern recognition receptors (PRRs) and cognate agonists responsible for inducing immune responses, and (iii) developments in nano- and microparticle fabrication and characterization techniques. Advances in particle engineering now allow highly tunable physicochemical properties of particle-based vaccines, including composition, size, shape, surface characteristics, and degradability. Enhanced collaborative efforts between researchers in immunology and materials science are expected to rise to next-generation vaccines. This process will be significantly aided by a greater understanding of the immunological principles guiding vaccine antigenicity, immunogenicity, and efficacy. With specific emphasis on PRR-targeted adjuvants and particle physicochemical properties, this review aims to provide an overview of the current literature to guide and focus rational particle-based vaccine design efforts.
Publisher: Royal Society of Chemistry (RSC)
Date: 2008
DOI: 10.1039/B712137G
Abstract: Fluorescent microcapsules doped with a europium beta-diketonate complex were fabricated for the first time by stepwise adsorption of polyelectrolytes and europium complex using the layer-by-layer technique. The influence of temperature and solvent treatment on the morphology of the microcapsules was investigated. Intense red light emission of the microcapsules could be clearly observed by fluorescence microscopy before and after treatment. Remarkable shrinking, decrease of the inner volume and increase of the wall thickness were observed using atomic force microscopy (AFM) and transmission electron microscopy (TEM) after thermal treatment. The shrinkage induced by annealing could be recovered by dissolving in ethanol solution, which was confirmed by AFM and TEM. Morphology variation of the luminescent microcapsules induced by annealing or solvent are both attributed to the molecular rearrangement of polyelectrolytes. While the shrinkage by annealing is an entropy driven process with formation of more coiled conformations of polyelectrolytes the morphology variation by ethanol might be due to the effective screening of electrostatic interaction within the polyelectrolyte multilayers and the changed interaction between hydrophobic fragments present in the polyelectrolytes.
Publisher: Wiley
Date: 25-04-2023
Abstract: Nanovaccine‐based immunotherapy can initiate strong immune responses and establish a long‐term immune memory to prevent tumor invasion and recurrence. Herein, the assembly of redox‐responsive antigen nanoparticles (NPs) conjugated with imidazoquinoline‐based TLR7/8 agonists for lymph node‐targeted immune activation is reported, which can potentiate tumor therapy and prevention. Antigen NPs are assembled via the templating of zeolitic imidazolate framework‐8 NPs to cross‐link ovalbumin with disulfide bonds, which enables the NPs with redox‐responsiveness for improved antigen cross‐presentation and dendritic cell activation. The formulated nanovaccines promote the lymphatic co‐delivery of antigens and agonists, which can trigger immune responses of cytotoxic T lymphocytes and strong immunological memory. Notably, nanovaccines demonstrate their superiority for tumor prevention owing to the elicited robust antitumor immunity. The reported strategy provides a rational design of nanovaccines for enhanced cancer immunotherapy.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1NR08114D
Abstract: We demonstrate an unusual state, the X state, by naturally drying up a dough which is composed of Ni(H 2 O) 2 [(Ni(CN) 4 ]·H 2 O nanosheets and water. This X-state mixture shows mechanical characteristics different from both liquids and brittle solids.
Publisher: American Chemical Society (ACS)
Date: 26-05-2017
DOI: 10.1021/ACS.BIOCONJCHEM.7B00168
Abstract: Particle-cell interactions are governed by, among other factors, the composition and surface properties of the particles. Herein, we report the preparation of various polymer capsules with different compositions and properties via atom transfer radical polymerization mediated continuous assembly of polymers (CAP
Publisher: American Chemical Society (ACS)
Date: 19-07-2019
Abstract: We report a facile inking strategy for visual information storage (e.g., writing, printing, and beyond) via surface modification of substrates with polyphenols and subsequent in situ formation of metal-phenolic networks (MPNs) on the substrates. The reported technique has several advantages compared with current printing techniques. Diverse substrates can be used to fulfill the requirements for different applications (e.g., printing, writing, painting, and st ing). A range of colors (e.g., yellow, blue, and green) can be realized using different polyphenols (e.g., tannic acid, gallic acid, and pyrogallol) and metal ions (e.g., Cu
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2MH00410K
Abstract: Self-reporting of damage in underwater materials allows on-demand maintenance and, therefore, improves the reliability of materials used in aquatic environments. Here, we report a chemiluminescence-based strategy to self-report the mechanical damage (
Publisher: American Chemical Society (ACS)
Date: 27-09-2022
DOI: 10.1021/JACS.2C06877
Abstract: Surface modification with poly(ethylene glycol) (PEGylation) is an effective strategy to improve the colloidal stability of nanoparticles (NPs) and is often used to minimize cellular uptake and clearance of NPs by the immune system. However, PEGylation can also trigger the accelerated blood clearance (ABC) phenomenon, which is known to reduce the circulation time of PEGylated NPs. Herein, we report the engineering of stealth PEG NPs that can avoid the ABC phenomenon and, when modified with hyaluronic acid (HA), show specific cancer cell targeting and drug delivery. PEG NPs cross-linked with disulfide bonds are prepared by using zeolitic imidazolate framework-8 NPs as templates. The reported templating strategy enables the simultaneous removal of the template and formation of PEG NPs under mild conditions (pH 5.5 buffer). Compared to PEGylated liposomes, PEG NPs avoid the secretion of anti-PEG antibodies and the presence of anti-PEG IgM and IgG did not significantly accelerate the blood clearance of PEG NPs, indicating the inhibition of the ABC effect for the PEG NPs. Functionalization of the PEG NPs with HA affords PEG NPs that retain their stealth properties against macrophages, target CD44-expressed cancer cells and, when loaded with the anticancer drug doxorubicin, effectively inhibit tumor growth. The innovation of this study lies in the engineering of PEG NPs that can circumvent the ABC phenomenon and that can be functionalized for the improved and targeted delivery of drugs.
Publisher: American Chemical Society (ACS)
Date: 27-09-2017
DOI: 10.1021/ACS.LANGMUIR.7B02692
Abstract: Metal-phenolic networks (MPNs) are a versatile class of self-assembled materials that are able to form functional thin films on various substrates with potential applications in areas including drug delivery and catalysis. Different metal ions (e.g., Fe
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5SC00416K
Abstract: A systematic and quantitative study on the role of capsule stiffness in cellular processing was performed using hyaluronic acid capsules with tunable stiffness constructed via continuous assembly of polymers.
Publisher: American Chemical Society (ACS)
Date: 30-09-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C0CC02680H
Abstract: Highly ordered freestanding honeycomb films with asymmetric through-pore structures were prepared from polystyrene/gold-nanoparticles (PS/AuNPs) nanocomposite at an air/water interface using a one-step interfacial self-assembly method.
Publisher: Wiley
Date: 24-08-2021
Abstract: We report a sono‐Fenton strategy to mediate the supramolecular assembly of metal–phenolic networks (MPNs) as substrate‐independent coatings using phenol and phenyl derivatives as building blocks. The assembly process is initiated from the generation of hydroxyl radicals ( . OH) using high‐frequency ultrasound (412 kHz), while the metal ions synergistically participate in the production of additional . OH for hydroxylation henolation of phenol and phenyl derivatives via the Fenton reaction and also coordinate with the phenolic compounds for film formation. The coating strategy is applicable to various phenol and phenyl derivatives and different metal ions including Fe II , Fe III , Cu II , and Co II . In addition, the sono‐Fenton strategy allows real‐time control over the assembly process by turning the high‐frequency ultrasound on or off. The properties of the building blocks are maintained in the formed films. This work provides an environmentally friendly and controllable method to expand the application of phenolic coatings for surface engineering.
Publisher: Royal Society of Chemistry (RSC)
Date: 2007
DOI: 10.1039/B701181D
Abstract: Rare-earth beta-diketone complex doped microcapsules with high efficiency fluorescence fabricated by the LbL technique based on electrostatic and charge-dipole interactions are reported.
Publisher: Elsevier BV
Date: 09-2022
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0CC03734F
Abstract: Scalable mineralization of zeolitic imidazolate framework-8 nanoparticles with versatility of cargo encapsulation and excellent colloidal dispersibility and stability is engineered using poly(ethylene glycol) as the mineralizer for therapeutic delivery.
Publisher: American Chemical Society (ACS)
Date: 08-2019
Abstract: In the present study, a capsule system that consists of a stealth carrier based on poly(ethylene glycol) (PEG) and functionalized with bispecific antibodies (BsAbs) is introduced to examine the influence of the capsule shape and size on cellular targeting. Hollow spherical and rod-shaped PEG capsules with tunable aspect ratios (ARs) of 1, 7, and 18 were synthesized and subsequently functionalized with BsAbs that exhibit dual specificities to PEG and epidermal growth factor receptor (EGFR). Dosimetry (variation between the concentrations of capsules present and capsules that reach the cell surface) was controlled through "dynamic" incubation (i.e., continuously mixing the incubation medium). The results obtained were compared with those obtained from the "static" incubation experiments. Regardless of the incubation method and the capsule shape and size studied, BsAb-functionalized PEG capsules showed >90% specific cellular association to EGFR-positive human breast cancer cells MDA-MB-468 and negligible association with both control cell lines (EGFR negative Chinese hamster ovary cells CHO-K1 and murine macrophages RAW 264.7) after incubation for 5 h. When dosimetry was controlled and the dose concentration was normalized to the capsule surface area, the size or shape had a minimal influence on the cell association behavior of the capsules. However, different cellular internalization behaviors were observed, and the capsules with ARs 7 and 18 were, respectively, the least and most optimal shape for achieving high cell internalization under both dynamic and static conditions. Dynamic incubation showed a greater impact on the internalization of rod-shaped capsules (∼58-67% change) than on the spherical capsules (∼24-29% change). The BsAb-functionalized PEG capsules reported provide a versatile particle platform for the evaluation and comparison of cellular targeting performance of capsules with different sizes and shapes in vitro.
Publisher: American Chemical Society (ACS)
Date: 19-10-2015
Publisher: American Chemical Society (ACS)
Date: 28-05-2015
DOI: 10.1021/ACS.LANGMUIR.5B01020
Abstract: Carbonic anhydrase (CA) is a native enzyme that facilitates the hydration of carbon dioxide into bicarbonate ions. This study reports the fabrication of thin films of active CA enzyme onto a porous membrane substrate using layer-by-layer (LbL) assembly. Deposition of multilayer films consisting of polyelectrolytes and CA was monitored by quartz crystal microgravimetry, while the enzymatic activity was assayed according to the rates of p-nitrophenylacetate (p-NPA) hydrolysis and CO2 hydration. The fabrication of the films onto a nonporous glass substrate showed CO2 hydration rates of 0.52 ± 0.09 μmol cm(-2) min(-1) per layer of bovine CA and 2.6 ± 0.7 μmol cm(-2) min(-1) per layer of a thermostable microbial CA. The fabrication of a multilayer film containing the microbial CA on a porous polypropylene membrane increased the hydration rate to 5.3 ± 0.8 μmol cm(-2) min(-1) per layer of microbial CA. The addition of mesoporous silica nanoparticles as a film layer prior to enzyme adsorption was found to increase the activity on the polypropylene membranes even further to a rate of 19 ± 4 μmol cm(-2) min(-1) per layer of microbial CA. The LbL treatment of these membranes increased the mass transfer resistance of the membrane but decreased the likelihood of membrane pore wetting. These results have potential application in the absorption of carbon dioxide from combustion flue gases into aqueous solvents using gas-liquid membrane contactors.
No related grants have been discovered for Jiwei Cui.