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

Abstract

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.

Authors:
 [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)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1185968
Grant/Contract Number:
AC05-00OR22725; DMR-1408811
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 7; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Bocharova, Vera, Sharp, Danna, Jones, Aaron, Cheng, Shiwang, Griffin, Philip J., Agapov, Alexander L., Voylov, Dmitry, Wang, Yangyang, Kisliuk, Alexander, Melman, Artem, and Sokolov, Alexei P. Enzyme Induced Formation of Monodisperse Hydrogel Nanoparticles Tunable in Size. United States: N. p., 2015. Web. doi:10.1021/acs.chemmater.5b00187.
Bocharova, Vera, Sharp, Danna, Jones, Aaron, Cheng, Shiwang, Griffin, Philip J., Agapov, Alexander L., Voylov, Dmitry, Wang, Yangyang, Kisliuk, Alexander, Melman, Artem, & Sokolov, Alexei P. Enzyme Induced Formation of Monodisperse Hydrogel Nanoparticles Tunable in Size. United States. doi:10.1021/acs.chemmater.5b00187.
Bocharova, Vera, Sharp, Danna, Jones, Aaron, Cheng, Shiwang, Griffin, Philip J., Agapov, Alexander L., Voylov, Dmitry, Wang, Yangyang, Kisliuk, Alexander, Melman, Artem, and Sokolov, Alexei P. Mon . "Enzyme Induced Formation of Monodisperse Hydrogel Nanoparticles Tunable in Size". United States. doi:10.1021/acs.chemmater.5b00187. https://www.osti.gov/servlets/purl/1185968.
@article{osti_1185968,
title = {Enzyme Induced Formation of Monodisperse Hydrogel Nanoparticles Tunable in Size},
author = {Bocharova, Vera and Sharp, Danna and Jones, Aaron and Cheng, Shiwang and Griffin, Philip J. and Agapov, Alexander L. and Voylov, Dmitry and Wang, Yangyang and Kisliuk, Alexander and Melman, Artem and Sokolov, Alexei P.},
abstractNote = {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.},
doi = {10.1021/acs.chemmater.5b00187},
journal = {Chemistry of Materials},
number = 7,
volume = 27,
place = {United States},
year = {Mon Mar 09 00:00:00 EDT 2015},
month = {Mon Mar 09 00:00:00 EDT 2015}
}

Journal Article:
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