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Blood Compatible Graphene/Heparin Conjugate through Noncovalent Chemistry

Blood compatible graphene/heparin conjugate is simply formulated through noncovalent interaction between chemically reduced graphene and heparin. Charge repulsion of negatively charged heparin on graphene plates renders hydrophobic graphene to be solublized in aqueous media without any precipitation or aggregation even after 6 months. Unfractioned heparin (UFH) with higher molecular weight was effective for graphene solubilization while low molecular weight heparin (LMWH) was not. Noncovalently interacting heparin chains on graphene plates preserve their anticoagulant activity after conjugation with graphene. Graphene/UFH conjugate shows much enhanced anti factor Xa (FXa) activity of 29.6 IU/mL compared with pristine graphene oxide (GO; 1.03 IU/mL).

Target Delivery and Cell Imaging Using Hyaluronic Acid-Functionalized Graphene Quantum Dots

This work demonstrates the way to achieve efficient and target specific delivery of a graphene quantum dot (GQD) using hyaluronic acid (HA) (GQD-HA) as a targeting agent. HA has been anchored to a GQD that accepts the fascinating adhesive properties of the catechol moiety, dopamine hydrochloride, conjugated to HA, which was confirmed by X-ray photoelectron spectroscopy. Transmission electron microscopy revealed a particle size of ∼20 nm, and the fluorescence spectra revealed significant fluorescence intensity even after the anchoring of HA. The prepared GQD-HA was applied to CD44 receptor overexpressed tumor-bearing balb/c female mice, and the in vivo biodistribution investigation demonstrated more bright fluorescence from the tumor tissue. In vitro cellular imaging, via a confocal laser scanning microscope, exhibited strong fluorescence from CD44 overexpressed A549 cells. Both in vivo and in vitro results showed the effectiveness of using HA as targeting molecule. The loading and release kinetics of the hydrophobic drug doxorubicin from a GQD under mildly acidic conditions showed that a GQD can be considered as a novel drug carrier, while the nontoxic behavior from the MTT assay strongly supports the identification of GQD-HA as a biocompatible material.

Optically modulated conduction in chromophore-functionalized single-wall carbon nanotubes

We demonstrate an optically active nanotube-hybrid material by functionalizing single-wall nanotubes with an azo-based chromophore. Upon UV illumination, the conjugated chromophore undergoes a cis-trans isomerization leading to a charge redistribution near the nanotube. This charge redistribution changes the local electrostatic environment, shifting the threshold voltage and increasing the conductivity of the nanotube transistor. For a approximately 1%-2% coverage, we measure a shift in the threshold voltage of up to 1.2 V. Further, the conductance change is reversible and repeatable over long periods of time, indicating that the chromophore-functionalized nanotubes are useful for integrated nanophotodetectors.

Additive-free hollow-structured Co3O4 nanoparticle Li-ion battery: the origins of irreversible capacity loss.

Origins of the irreversible capacity loss were addressed through probing changes in the electronic and structural properties of hollow-structured Co3O4 nanoparticles (NPs) during lithiation and delithiation using electrochemical Co3O4 transistor devices that function as a Co3O4 Li-ion battery. Additive-free Co3O4 NPs were assembled into a Li-ion battery, allowing us to isolate and explore the effects of the Co and Li2O formation/decomposition conversion reactions on the electrical and structural degradation within Co3O4 NP films. NP films ranging between a single monolayer and multilayered film hundreds of nanometers thick prepared with blade-coating and electrophoretic deposition methods, respectively, were embedded in the transistor devices for in situ conduction measurements as a function of battery cycles. During battery operation, the electronic and structural properties of Co3O4 NP films in the bulk, Co3O4/electrolyte, and Co3O4/current collector interfaces were spatially mapped to address the origin of the initial irreversible capacity loss from the first lithiation process. Further, change in carrier injection/extraction between the current collector and the Co3O4 NPs was explored using a modified electrochemical transistor device with multiple voltage probes along the electrical channel.

Recyclable and stable silver deposited magnetic nanoparticles with poly (vinyl pyrrolidone)-catechol coated iron oxide for antimicrobial activity.

This paper introduces a facile method to make highly stable and recyclable antimicrobial magnetic nanoparticles (NPs). Initially, magnetic iron oxide nanoparticles (IONPs) were coated with poly (vinyl pyrrolidone) conjugated catechol (PVP-CCDP). Afterward, silver nanoparticles (Ag(0)) were deposited onto PVP-CCDP coated IONPs using remain catechol. The prepared nanoparticles showed long term (~4 weeks) colloidal stability and redispersibility, respectively, against external magnetic field and over a broad range of pH (4-12). The NPs were characterized by UV-vis, SEM, XPS, and XRD measurements. TEM and DLS analyses showed that the mean particle size of PVP-CCDP coated IONPs/Ag(0) were about 72 nm. The recyclable magnetic NPs possessed a high antibacterial effect against the model microbes Staphylococcus aureus and Escherichia coli and could be separated easily using magnet following antibacterial test for repeated uses and maintained 100% antibacterial efficiency during three cycles. In MTT assay, the magnetic nanoparticles possessed no measureable cytotoxicity to live cells.

Target delivery of β-cyclodextrin/paclitaxel complexed fluorescent carbon nanoparticles: externally NIR light and internally pH sensitive-mediated release of paclitaxel with bio-imaging

The development of cooperative drug delivery systems that can detect and target the disease site, with rapid trigger controlled drug release (internally and externally), is widely expected to change the landscape of future drug carriers. In this study a drug delivery system was developed for the cancer-targeted release of chemotherapeutic agents inside living cells. This system is an environment sensitive (pH), and external photothermally remote controlled, cooperative image-guided drug delivery matrix. Partially carbonized fluorescence hyaluronic acid (HA-FCN) was conjugated with boronic acid (BA) to promote the formation of boronate ester with diol groups of β-cyclodextrin (CD) [HA-FCN-CD]. The pH influence mediated release of paclitaxel (PTX) from the CD cavity of HA-FCN-CD was utilized for targeted cancer bioimaging. This active-target delivery system (HA-FCN-CD-PTX) was found to show optical absorption properties similar to those of the near infrared (NIR) light sensitive carbonized material. This system exploits acidity for triggered drug release and rapid generation of mild photothermal heat to trigger burst release of PTX. Cooperative guided bioimaging that employs both internal pH responsive and external NIR controlled drug carriers is a promising method for chemotherapeutic release that can be adjusted according to physiological needs.

In Vitro and In Vivo Tumor Targeted Photothermal Cancer Therapy Using Functionalized Graphene Nanoparticles

Despite the tremendous progress that photothermal therapy (PTT) has recently achieved, it still has a long way to go to gain the effective targeted photothermal ablation of tumor cells. Driven by this need, we describe a new class of targeted photothermal therapeutic agents for cancer cells with pH responsive bioimaging using near-infrared dye (NIR) IR825, conjugated poly(ethylene glycol)-g-poly(dimethylaminoethyl methacrylate) (PEG-g-PDMA, PgP), and hyaluronic acid (HA) anchored reduced graphene oxide (rGO) hybrid nanoparticles. The obtained rGO nanoparticles (PgP/HA-rGO) showed pH-dependent fluorescence emission and excellent near-infrared (NIR) irradiation of cancer cells targeted in vitro to provide cytotoxicity. Using intravenously administered PTT agents, the time-dependent in vivo tumor target accumulation was exactly defined, presenting eminent photothermal conversion at 4 and 8 h post-injection, which was demonstrated from the ex vivo biodistribution of tumors. These tumor environment responsive hybrid nanoparticles generated photothermal heat, which caused dominant suppression of tumor growth. The histopathological studies obtained by H&E staining demonstrated complete healing from malignant tumor. In an area of limited successes in cancer therapy, our translation will pave the road to design stimulus environment responsive targeted PTT agents for the safe eradication of devastating cancer.

Iron Oxide@PEDOT-Based Recyclable Photothermal Nanoparticles with Poly(vinylpyrrolidone) Sulfobetaines for Rapid and Effective Antibacterial Activity.

Growing microbial resistance that renders antibiotic treatment vulnerable has emerged, attracting a great deal of interest in the need to develop alternative antimicrobial treatments. To contribute to this effort, we report magnetic iron oxide (Fe3O4) nanoparticles (NPs) coated with catechol-conjugated poly(vinylpyrrolidone) sulfobetaines (C-PVPS). This negatively charged Fe3O4@C-PVPS is subsequently encapsulated by poly(3,4-ethylenedioxythiophene) (PEDOT) following a layer-by-layer (LBL) self-assembly method. The obtained Fe3O4@C-PVPS:PEDOT nanoparticles appear to be novel NIR-irradiated photothermal agents that can achieve effective bacterial killing and are reusable after isolation of the used particles using external magnetic fields. The recyclable Fe3O4@C-PVPS:PEDOT NPs exhibit a high efficiency in converting photothermal heat for rapid antibacterial effects against Staphylococcus aureus and Escherichia coli. In this study, antibacterial tests for repeated uses maintained almost 100% antibacterial efficiency during three cycles and provided rapid and effective killing of 99% Gram-positive and -negative bacteria within 5 min of near-infrared (NIR) light exposure. The core-shell nanoparticles (Fe3O4@C-PVPS:PEDOT) exhibit the required stability, and their paramagnetic nature means that they rapidly convert photothermal heat sufficient for use as NIR-irradiated antibacterial photothermal sterilizing agents.

Light Controllable Surface Coating for Effective Photothermal Killing of Bacteria

Although the electronic properties of conducting films have been widely explored in optoelectronic fields, the optical absorption abilities of surface-coated films for photothermal conversion have been relatively less explored in the production of antibacterial coatings. Here, we present catechol-conjugated poly(vinylpyrrolidone) sulfobetaine (PVPS) and polyaniline (PANI) tightly linked by ionic interaction (PVPS:PANI) as a novel photothermal antibacterial agent for surface coating, which can absorb broadband near-infrared (NIR) light. Taking advantage of the NIR light absorption, this coating film can release eminent photothermal heat for the rapid killing of surface bacteria. The NIR light triggers a sharp rise in photothermal heat, providing the rapid and effective killing of 99.9% of the Gram-positive and -negative bacteria tested within 3 min of NIR light exposure when used at the concentration of 1 mg/mL. Although considerable progress has been made in the design of antibacterial coatings, the user control of NIR-irradiated rapid photothermal destruction of surface bacteria holds increasing attention beyond the traditional boundaries of typical antibacterial surfaces.

Photo- and pH-Tunable Multicolor Fluorescent Nanoparticle-Based Spiropyran- and BODIPY-Conjugated Polymer with Graphene Oxide

We report a stimuli-responsive fluorescent nanomaterial, based on graphene oxide coupled with a polymer conjugated with photochromic spiropyran (SP) dye and hydrophobic boron dipyrromethane (BODIPY) dye, for application in triggered target multicolor bioimaging. Graphene oxide (GO) was reduced by catechol-conjugated polymers under mildly alkaline conditions, which enabled to formation of functionalized multicolor graphene nanoparticles that can be induced by irradiation with UV light and by changing the pH from acidic to neutral. Investigation of these nanoparticles by using AFM, fluorescence emission, and in vitro cell and in vivo imaging revealed that they show different tunable colors in bioimaging applications and, more specifically, in cancer-cell detection. The stability, biocompatibility, and quenching efficacy of this nanocomposite open a different perspective for cell imaging in different independent colors, sequentially and simultaneously.