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Title: Structurally colored protease responsive nanoparticle hydrogels with degradation-directed assembly

Abstract

A tunable protease responsive nanoparticle hydrogel (PRNH) that demonstrates large non-iridescent color changes due to a degradation-directed assembly of nanoparticles is reported. Structurally colored composites are fabricated with silica particles, 4-arm poly(ethylene glycol) norbornene (4PEGN), and a proteolytically degradable peptide. When placed in a protease solution, the peptide crosslinks degrade causing electrostatic binding and adsorption of the polymer to the particle surface which leads to the assembly of particles into compact amorphous arrays with structural color. The particle surface charge and size is investigated to probe their effect on the assembly mechanism. Interestingly, only PRNHs with highly negative particle surface charge exhibit color changes after degradation. Ultra-small angle X-ray scattering revealed that the particles become coated in polymer after degradation, producing a material with less order compared to the initial state. Altering the particle diameter modulates the composites’ color, and all sizes investigated (178–297 nm) undergo the degradation-directed assembly. Varying the amount of 4PEGN adjusts the swollen PRNH color and has no effect on the degradation-directed assembly. Finally, taken together, the effects of surface charge, particle size, and polymer concentration allow for the formulation of new design rules for fabricating tunable PRNHs that display vivid changes in structural color uponmore » degradation.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [1];  [1];  [2];  [3];  [1]; ORCiD logo [1]
  1. Univ. of Maryland, College Park, MD (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). X-Ray Sciences Division
  3. Univ. of New South Wales, Sydney, NSW (Australia)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); National Institutes of Health (NIH) - National Institute of Biomedical Imaging and Bioengineering (NIBIB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1616158
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 11; Journal Issue: 38; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Torres, Leopoldo, Daristotle, John L., Ayyub, Omar B., Bellato Meinhardt, Bianca M., Garimella, Havisha, Margaronis, Artemis, Seifert, Soenke, Bedford, Nicholas M., Woehl, Taylor J., and Kofinas, Peter. Structurally colored protease responsive nanoparticle hydrogels with degradation-directed assembly. United States: N. p., 2019. Web. https://doi.org/10.1039/c9nr04624k.
Torres, Leopoldo, Daristotle, John L., Ayyub, Omar B., Bellato Meinhardt, Bianca M., Garimella, Havisha, Margaronis, Artemis, Seifert, Soenke, Bedford, Nicholas M., Woehl, Taylor J., & Kofinas, Peter. Structurally colored protease responsive nanoparticle hydrogels with degradation-directed assembly. United States. https://doi.org/10.1039/c9nr04624k
Torres, Leopoldo, Daristotle, John L., Ayyub, Omar B., Bellato Meinhardt, Bianca M., Garimella, Havisha, Margaronis, Artemis, Seifert, Soenke, Bedford, Nicholas M., Woehl, Taylor J., and Kofinas, Peter. Mon . "Structurally colored protease responsive nanoparticle hydrogels with degradation-directed assembly". United States. https://doi.org/10.1039/c9nr04624k. https://www.osti.gov/servlets/purl/1616158.
@article{osti_1616158,
title = {Structurally colored protease responsive nanoparticle hydrogels with degradation-directed assembly},
author = {Torres, Leopoldo and Daristotle, John L. and Ayyub, Omar B. and Bellato Meinhardt, Bianca M. and Garimella, Havisha and Margaronis, Artemis and Seifert, Soenke and Bedford, Nicholas M. and Woehl, Taylor J. and Kofinas, Peter},
abstractNote = {A tunable protease responsive nanoparticle hydrogel (PRNH) that demonstrates large non-iridescent color changes due to a degradation-directed assembly of nanoparticles is reported. Structurally colored composites are fabricated with silica particles, 4-arm poly(ethylene glycol) norbornene (4PEGN), and a proteolytically degradable peptide. When placed in a protease solution, the peptide crosslinks degrade causing electrostatic binding and adsorption of the polymer to the particle surface which leads to the assembly of particles into compact amorphous arrays with structural color. The particle surface charge and size is investigated to probe their effect on the assembly mechanism. Interestingly, only PRNHs with highly negative particle surface charge exhibit color changes after degradation. Ultra-small angle X-ray scattering revealed that the particles become coated in polymer after degradation, producing a material with less order compared to the initial state. Altering the particle diameter modulates the composites’ color, and all sizes investigated (178–297 nm) undergo the degradation-directed assembly. Varying the amount of 4PEGN adjusts the swollen PRNH color and has no effect on the degradation-directed assembly. Finally, taken together, the effects of surface charge, particle size, and polymer concentration allow for the formulation of new design rules for fabricating tunable PRNHs that display vivid changes in structural color upon degradation.},
doi = {10.1039/c9nr04624k},
journal = {Nanoscale},
number = 38,
volume = 11,
place = {United States},
year = {2019},
month = {9}
}

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