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Title: Enzyme Induced Formation of Monodisperse Hydrogel Nanoparticles Tunable in Size

Journal Article · · Chemistry of Materials
 [1];  [2];  [2];  [1];  [3];  [2];  [2];  [1];  [1];  [4];  [5]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Univ. of Pennsylvania, Philadelphia, PA (United States)
  4. Clarkson Univ., Potsdam, NY (United States)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Here, we report a novel approach to synthesize monodisperse hydrogel nanoparticles that are tunable in size. The distinctive feature of our approach is the use of a multicopper oxidase enzyme, laccase, as both a biocatalyst and template for nanoparticle growth. We utilize the ferroxidase activity of laccase to initiate localized production of iron(III) cations from the oxidation of iron(II) cations. We demonstrate that nanoparticles are formed in a dilute polymer solution of alginate as a result of cross-linking between alginate and enzymatically produced iron(III) cations. Exerting control over the enzymatic reaction allows for nanometer-scale tuning of the hydrogel nanoparticle radii in the range of 30–100 nm. Moreover, the nanoparticles and their growth kinetics were characterized via dynamic light scattering, atomic force microscopy, and UV–vis spectroscopy. Our finding opens up a new avenue for the synthesis of tunable nanoscale hydrogel particles for biomedical applications.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725; DMR-1408811
OSTI ID:
1185968
Journal Information:
Chemistry of Materials, Vol. 27, Issue 7; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 9 works
Citation information provided by
Web of Science

References (43)

A Solvent-Free Thermosponge Nanoparticle Platform for Efficient Delivery of Labile Proteins journal October 2014
Lipopeptide nanoparticles for potent and selective siRNA delivery in rodents and nonhuman primates journal February 2014
Multifunctional Inorganic Nanoparticles for Imaging, Targeting, and Drug Delivery journal May 2008
Gold Nanoparticles: A Revival in Precious Metal Administration to Patients journal October 2011
Effects of Particle Size and Surface Modification on Cellular Uptake and Biodistribution of Polymeric Nanoparticles for Drug Delivery journal January 2013
Nanoparticle therapeutics: an emerging treatment modality for cancer journal September 2008
Assessing Nanoparticle Toxicity journal July 2012
Strategies in the design of nanoparticles for therapeutic applications journal July 2010
Biocompatibility of engineered nanoparticles for drug delivery journal March 2013
The development of microgels/nanogels for drug delivery applications journal April 2008
Nanogels as Pharmaceutical Carriers: Finite Networks of Infinite Capabilities journal July 2009
Self-assembled Nanogel Engineering for Advanced Biomedical Technology journal March 2012
Self-aggregates of hydrophobized polysaccharides in water. Formation and characteristics of nanoparticles journal June 1993
Microscopic Structure and Thermoresponsiveness of a Hydrogel Nanoparticle by Self-Assembly of a Hydrophobized Polysaccharide journal February 1997
Structural Determination and Interior Polarity of Self-Aggregates Prepared from Deoxycholic Acid-Modified Chitosan in Water journal January 1998
Aggregation in Water of Dextran Hydrophobically Modified with Bile Acids journal October 1999
Self-Assembled Nanogel of Hydrophobized Dendritic Dextrin for Protein Delivery journal July 2009
Biodegradable Nanogel Formation of Polylactide-Grafted Dextran Copolymer in Dilute Aqueous Solution and Enhancement of Its Stability by Stereocomplexation journal July 2007
Self-Cross-Linked Polymer Nanogels: A Versatile Nanoscopic Drug Delivery Platform journal December 2010
Surfactant-Free Synthesis of Biodegradable, Biocompatible, and Stimuli-Responsive Cationic Nanogel Particles journal September 2013
Release dynamics of ciprofloxacin from swellable nanocarriers of poly(2-hydroxyethyl methacrylate): an in vitro study journal June 2010
pH sensitive swelling and releasing behavior of nano-gels based on polyaspartamide graft copolymers journal April 2011
Lidocaine loaded biodegradable nanospheres journal August 1999
Synthesis and Characterizations of In Situ Cross-Linkable Gelatin and 4-Arm-PPO-PEO Hybrid Hydrogels via Enzymatic Reaction for Tissue Regenerative Medicine journal February 2012
Enzyme-mediated fast in situ formation of hydrogels from dextran–tyramine conjugates journal January 2007
Tailorable Cell Culture Platforms from Enzymatically Cross-Linked Multifunctional Poly(ethylene glycol)-Based Hydrogels journal January 2013
Enzymatically Crosslinked Dextran-Tyramine Hydrogels as Injectable Scaffolds for Cartilage Tissue Engineering journal August 2010
In Situ Forming Hydrogels Based on Tyramine Conjugated 4-Arm-PPO-PEO via Enzymatic Oxidative Reaction journal February 2010
Multicopper oxidase-1 is a ferroxidase essential for iron homeostasis in Drosophila melanogaster journal July 2012
Multi-Copper Oxidases and Human Iron Metabolism journal June 2013
Electrochemically Controlled Drug-Mimicking Protein Release from Iron-Alginate Thin-Films Associated with an Electrode journal January 2012
Electrochemically stimulated release of lysozyme from an alginate matrix cross-linked with iron cations journal January 2012
Photodegradable Iron(III) Cross-Linked Alginate Gels journal July 2012
A Study of the Chain Stiffness and Extension of Alginates, in Vitro Epimerized Alginates, and Periodate-Oxidized Alginates Using Size-Exclusion Chromatography Combined with Light Scattering and Viscosity Detectors journal July 2006
Dioxygen Reactivity of Laccase: Dependence on Laccase Source, pH, and Anion Inhibition journal January 2001
Preparation of Ionically Cross-Linked Pectin Nanoparticles in the Presence of Chlorides of Divalent and Monovalent Cations journal September 2013
Enzyme Kinetics book January 2008
Enzymatically Cross-Linked Hyperbranched Polyglycerol Hydrogels as Scaffolds for Living Cells journal October 2014
Crystal Structure of a Laccase from the Fungus Trametes versicolor at 1.90-Å Resolution Containing a Full Complement of Coppers journal August 2002
Isolation and structural analysis of the laccase gene from the ligninegrading fungus Phlebia radiata journal July 1991
Characterization and structural analysis of the laccase I gene from the newly isolated ligninolytic basidiomycete PM1 (CECT 2971) journal December 1993
Effect of Ca 2+ , Ba 2+ , and Sr 2+ on Alginate Microbeads journal April 2006
Reexamining the Egg-Box Model in Calcium−Alginate Gels with X-ray Diffraction journal February 2007

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