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Title: Chitosan-Gated Magnetic-Responsive Nanocarrier for Dual-Modal Optical Imaging, Switchable Drug Release, and Synergistic Therapy

Abstract

In this study, we present a multifunctional yet structurally simple nanocarrier that has a high drug loading capacity, releases drug in response to onset of an AC magnetic field, and can serve as a long-term imaging contrast agent and effectively kills cancer cells by synergistic action. This nanocarrier (HMMC-NC) has a spherical shell structure with a center cavity of 80 nm in diameter. The shell is comprised of two layers: an inner layer of magnetite that exhibits superparamagnetism and an outer layer of mesoporous carbon embedded with carbon dots that exhibit photoluminescence property. Thus in addition to being a drug carrier, HMMC-NC is also a contrast agent for bioimaging. The switchable drug release is enabled by the chitosan molecules attached on the nanocarrier as the switching material which turns on or off the drug release in response to the application or withdrawal of an AC magnetic field.

Authors:
 [1];  [1];  [1];  [1];  [1];  [2];  [3];  [1]
  1. Department of Materials Science and Engineering, University of Washington, Seattle WA 98195 USA
  2. Department of Materials Science and Engineering, University of Washington, Seattle WA 98195 USA; Fundamental and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland WA 99354 USA
  3. Department of Chemistry, The College of Staten Island, City University of New York, Staten Island NY 10314 USA
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1361983
Report Number(s):
PNNL-SA-126395
Journal ID: ISSN 2192-2640
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Advanced Healthcare Materials; Journal Volume: 6; Journal Issue: 6
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 60 APPLIED LIFE SCIENCES

Citation Formats

Wang, Hui, Mu, Qingxin, Revia, Richard, Wang, Kui, Zhou, Xuezhe, Pauzauskie, Peter J., Zhou, Shuiqin, and Zhang, Miqin. Chitosan-Gated Magnetic-Responsive Nanocarrier for Dual-Modal Optical Imaging, Switchable Drug Release, and Synergistic Therapy. United States: N. p., 2017. Web. doi:10.1002/adhm.201601080.
Wang, Hui, Mu, Qingxin, Revia, Richard, Wang, Kui, Zhou, Xuezhe, Pauzauskie, Peter J., Zhou, Shuiqin, & Zhang, Miqin. Chitosan-Gated Magnetic-Responsive Nanocarrier for Dual-Modal Optical Imaging, Switchable Drug Release, and Synergistic Therapy. United States. doi:10.1002/adhm.201601080.
Wang, Hui, Mu, Qingxin, Revia, Richard, Wang, Kui, Zhou, Xuezhe, Pauzauskie, Peter J., Zhou, Shuiqin, and Zhang, Miqin. Wed . "Chitosan-Gated Magnetic-Responsive Nanocarrier for Dual-Modal Optical Imaging, Switchable Drug Release, and Synergistic Therapy". United States. doi:10.1002/adhm.201601080.
@article{osti_1361983,
title = {Chitosan-Gated Magnetic-Responsive Nanocarrier for Dual-Modal Optical Imaging, Switchable Drug Release, and Synergistic Therapy},
author = {Wang, Hui and Mu, Qingxin and Revia, Richard and Wang, Kui and Zhou, Xuezhe and Pauzauskie, Peter J. and Zhou, Shuiqin and Zhang, Miqin},
abstractNote = {In this study, we present a multifunctional yet structurally simple nanocarrier that has a high drug loading capacity, releases drug in response to onset of an AC magnetic field, and can serve as a long-term imaging contrast agent and effectively kills cancer cells by synergistic action. This nanocarrier (HMMC-NC) has a spherical shell structure with a center cavity of 80 nm in diameter. The shell is comprised of two layers: an inner layer of magnetite that exhibits superparamagnetism and an outer layer of mesoporous carbon embedded with carbon dots that exhibit photoluminescence property. Thus in addition to being a drug carrier, HMMC-NC is also a contrast agent for bioimaging. The switchable drug release is enabled by the chitosan molecules attached on the nanocarrier as the switching material which turns on or off the drug release in response to the application or withdrawal of an AC magnetic field.},
doi = {10.1002/adhm.201601080},
journal = {Advanced Healthcare Materials},
number = 6,
volume = 6,
place = {United States},
year = {Wed Jan 25 00:00:00 EST 2017},
month = {Wed Jan 25 00:00:00 EST 2017}
}
  • In our paper reports a type of multifunctional hybrid nanoparticle (NP) composed of gold nanocrystals coated on and/or embedded in a magnetite-fluorescent porous carbon core-shell NP template (Fe 3O 4@PC-CDs-Au) for biomedical applications, including magnetic/NIR-responsive drug release, multicolor cell imaging, and enhanced photothermal therapy. The synthesis of the Fe 3O 4@PC-CDs-Au NPs firstly involves the preparation of core-shell template NPs with magnetite nanocrystals clustered in the cores and fluorescent carbon dots (CDs) embedded in a porous carbon shell, followed by an in situ reduction of silver ions (Ag +) loaded in the porous carbon shell and a subsequent replacement ofmore » Ag NPs with Au NPs through a galvanic replacement reaction using HAuCl 4 as a precursor. Moreover, the Fe 3O 4@PC-CDsAu NPs can enter the intracellular region and light up mouse melanoma B16F10 cells in multicolor mode. The porous carbon shell, anchored with hydrophilic hydroxyl/carboxyl groups, endows the Fe 3O 4@PC-CDs-Au NPs with excellent stability in the aqueous phase and a high loading capacity (719 mg g -1) for the anti-cancer drug doxorubicin (DOX). The superparamagnetic Fe 3O 4@PC-CDs-Au NPs with a saturation magnetization of 23.26 emu g -1 produce localized heat under an alternating magnetic field, which triggers the release of the loaded drug. The combined photothermal effects of the Au nanocrystals and the CDs on/in the carbon shell can not only regulate the release rate of the loaded drug, but also efficiently kill tumor cells under NIR irradiation. Finally, in benefitting from their excellent optical properties, their magnetic field and NIR light-responsive drug release capabilities and their enhanced photothermal effect, such nanostructured Fe 3O 4@PC-CDs-Au hybrid NPs are very promising for simultaneous imaging diagnostics and high efficacy therapy.« less
  • Remotely optical sensing and drug delivery using an environmentally-guided magnetically-driven hybrid nanogel particle could allow for medical diagnostics and treatment. Such multifunctional hybrid nanogels (<200 nm) were prepared through the first synthesis of magnetic Ni NPs, followed by a moderate growth of fluorescent metallic Ag on the surface of Ni NPs, and then a coverage of a pH-responsive copolymer gel shell of poly(ethylene glycol-co-methacrylic acid) [p(EG-MAA)] onto the Ni-Ag bimetallic NP cores (18 {+-} 5 nm). The introduction of the pH-responsive p(EG-MAA) gel shell onto the magnetic and fluorescent Ni-Ag NPs makes the polymer-bound Ni-Ag NPs responsive to pH overmore » the physiologically important range 5.0-7.4. The hybrid nanogels can adapt to surrounding pH and regulate the sensitivity in response to external magnetic field (such as a small magnet of 0.1 T), resulting in the accumulation of the hybrid nanogels within the duration from hours to a few seconds as the pH value decreases from 7.4 to 5.0. The pH-dependent magnetic response characteristic of the hybrid nanogels were further integrated with the pH change to fluorescent signal transduction and pH-regulated anticancer drug (a model drug 5-fluorouracil) delivery functions. The hybrid nanogels can overcome cellular barriers to enter the intracellular region and light up the mouse melanoma B16F10 cells. The multiple responsive hybrid nanogel that can be manipulated in tandem endogenous and exogenous activation should enhance our ability to address the complexity of biological systems.« less
  • A hybrid temperature-responsive hydroxyapatite-poly(N-isopropylacrylamide) (HAP-PNIPAAm) gel has been synthesized by the interpenetration of PNIPAAm into a sintered HAP disk through a radical-initiated polymerization of NIPAAm monomers under N2 atmosphere, and shows sustained positive thermo-responsive drug release profile over a month at PBS buffer.
  • A temperature-responsive composite based on poly (N-isopropylacrylamide) (PNIPAAm) and ordered mesoporous carbons (OMCs) has been successfully prepared by a simple wetness impregnation technique. The structures and properties of the composite were characterized by infrared spectroscopy (IR), X-ray diffraction (XRD), transmission electron microscopy (TEM), N{sub 2} sorption, thermogravimetric analysis (TG) and differential scanning calorimetry (DSC). The results showed that the inclusion of PNIPAAm had not greatly changed the basic ordered pore structure of the OMCs. Ibuprofen (IBU) was selected as model drug, and in vitro test of IBU release exhibited a temperature-responsive controlled release delivery. - Graphical abstract: The bands locatedmore » at 1650 and 1549 cm{sup -1} could be assigned to C=O stretching and N-H bending vibrations for polymer PNIPAAm (a). The bands at 1388 and 1369 cm{sup -1} were due to isopropyl group, and the band at 1459 cm{sup -1} was related to the bending vibration of C-H (a). For the PNIPAAm/OMCs composite, the characteristic bands of polymer were still observed besides those for carbon materials and the bands at around 1585 cm{sup -1} and a broad band at about 1100 cm{sup -1} were characteristics for the carbon materials(c). In addition, little shifts of C=O and N-H bands compared to the pure PNIPAAm were also observed (b), indicating a weak interaction between the polymer and carbon material. These results could be a proof that the PNIPAAm has been incorporated into the carbon material. Highlights: > A temperature-responsive PNIPAAm/OMCs composite was successfully synthesized by a simple wetness impregnation technique for the first time. > The inclusion of PNIPAAm had not greatly changed the basic ordered pore structure of the OMCs. > In vitro test of IBU release exhibited a temperature-responsive controlled release delivery.« less