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Title: Unusual multiscale mechanics of biomimetic nanoparticle hydrogels

Viscoelastic properties are central for gels and other materials. Simultaneously, high storage and loss moduli are difficult to attain due to their contrarian requirements to chemical structure. Biomimetic inorganic nanoparticles offer a promising toolbox for multiscale engineering of gel mechanics, but a conceptual framework for their molecular, nanoscale, mesoscale, and microscale engineering as viscoelastic materials is absent. Here we show nanoparticle gels with simultaneously high storage and loss moduli from CdTe nanoparticles. Viscoelastic figure of merit reaches 1.83 MPa exceeding that of comparable gels by 100–1000 times for glutathione-stabilized nanoparticles. The gels made from the smallest nanoparticles display the highest stiffness, which was attributed to the drastic change of GSH configurations when nanoparticles decrease in size. A computational model accounting for the difference in nanoparticle interactions for variable GSH configurations describes the unusual trends of nanoparticle gel viscoelasticity. These observations are generalizable to other NP gels interconnected by supramolecular interactions and lead to materials with high-load bearing abilities and energy dissipation needed for multiple technologies.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [3] ;  [7] ;  [7] ;  [7] ;  [6] ;  [8] ;  [3] ;  [9] ; ORCiD logo [10]
  1. Wenzhou Medical Univ. (China). School of Biomedical Engineering. School of Ophthalmology and Optometry. Eye Hospital; Chinese Academy of Sciences (CAS), Wenzhou (China). Wenzhou Inst. of Biomaterials and Engineering; Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering. Biointerfaces Inst.
  2. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering. Biointerfaces Inst.; Univ. of California, San Francisco, CA (United States). Dept. of Cellular and Molecular Pharmacology
  3. Univ. of Michigan, Ann Arbor, MI (United States). Biophysics. Dept. of Chemistry
  4. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering. Biointerfaces Inst.; Friedrich-Alexander Univ. Erlangen-Nurnberg, Erlangen (Germany). Inst. for Multiscale Simulation
  5. Wenzhou Medical Univ. (China). School of Biomedical Engineering. School of Ophthalmology and Optometry. Eye Hospital
  6. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering. Biointerfaces Inst.
  7. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Materials Science and Engineering
  8. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Materials Science and Engineering; National Renewable Energy Lab. (NREL), Golden, CO (United States)
  9. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering. Biointerfaces Inst. Dept. of Materials Science and Engineering
  10. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering. Biointerfaces Inst. Dept. of Materials Science and Engineering. Dept. of Biomedical Engineering; Michigan Center for Integrative Research in Critical Care (MCIRC), Ann Arbor, MI (United States)
Publication Date:
Report Number(s):
NREL/JA-5A00-71024
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC36-08GO28308; W911NF-10-1-0518; EFRI-BSBA 0938019; DMR 1120923; CBET 1036672; CBET 1403777; DMR 1411014; 21573162; 21773172; WIBEZD2014001-02
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Univ. of Michigan, Ann Arbor, MI (United States); Wenzhou Medical Univ. (China); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE; US Army Research Office (ARO); National Science Foundation (NSF); National Natural Science Foundation of China (NNSFC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; gels and hydrogels; nanoparticles; self-assembly
OSTI Identifier:
1423556

Zhou, Yunlong, Damasceno, Pablo F., Somashekar, Bagganahalli S., Engel, Michael, Tian, Falin, Zhu, Jian, Huang, Rui, Johnson, Kyle, McIntyre, Carl, Sun, Kai, Yang, Ming, Green, Peter F., Ramamoorthy, Ayyalusamy, Glotzer, Sharon C., and Kotov, Nicholas A.. Unusual multiscale mechanics of biomimetic nanoparticle hydrogels. United States: N. p., Web. doi:10.1038/s41467-017-02579-w.
Zhou, Yunlong, Damasceno, Pablo F., Somashekar, Bagganahalli S., Engel, Michael, Tian, Falin, Zhu, Jian, Huang, Rui, Johnson, Kyle, McIntyre, Carl, Sun, Kai, Yang, Ming, Green, Peter F., Ramamoorthy, Ayyalusamy, Glotzer, Sharon C., & Kotov, Nicholas A.. Unusual multiscale mechanics of biomimetic nanoparticle hydrogels. United States. doi:10.1038/s41467-017-02579-w.
Zhou, Yunlong, Damasceno, Pablo F., Somashekar, Bagganahalli S., Engel, Michael, Tian, Falin, Zhu, Jian, Huang, Rui, Johnson, Kyle, McIntyre, Carl, Sun, Kai, Yang, Ming, Green, Peter F., Ramamoorthy, Ayyalusamy, Glotzer, Sharon C., and Kotov, Nicholas A.. 2018. "Unusual multiscale mechanics of biomimetic nanoparticle hydrogels". United States. doi:10.1038/s41467-017-02579-w. https://www.osti.gov/servlets/purl/1423556.
@article{osti_1423556,
title = {Unusual multiscale mechanics of biomimetic nanoparticle hydrogels},
author = {Zhou, Yunlong and Damasceno, Pablo F. and Somashekar, Bagganahalli S. and Engel, Michael and Tian, Falin and Zhu, Jian and Huang, Rui and Johnson, Kyle and McIntyre, Carl and Sun, Kai and Yang, Ming and Green, Peter F. and Ramamoorthy, Ayyalusamy and Glotzer, Sharon C. and Kotov, Nicholas A.},
abstractNote = {Viscoelastic properties are central for gels and other materials. Simultaneously, high storage and loss moduli are difficult to attain due to their contrarian requirements to chemical structure. Biomimetic inorganic nanoparticles offer a promising toolbox for multiscale engineering of gel mechanics, but a conceptual framework for their molecular, nanoscale, mesoscale, and microscale engineering as viscoelastic materials is absent. Here we show nanoparticle gels with simultaneously high storage and loss moduli from CdTe nanoparticles. Viscoelastic figure of merit reaches 1.83 MPa exceeding that of comparable gels by 100–1000 times for glutathione-stabilized nanoparticles. The gels made from the smallest nanoparticles display the highest stiffness, which was attributed to the drastic change of GSH configurations when nanoparticles decrease in size. A computational model accounting for the difference in nanoparticle interactions for variable GSH configurations describes the unusual trends of nanoparticle gel viscoelasticity. These observations are generalizable to other NP gels interconnected by supramolecular interactions and lead to materials with high-load bearing abilities and energy dissipation needed for multiple technologies.},
doi = {10.1038/s41467-017-02579-w},
journal = {Nature Communications},
number = ,
volume = 9,
place = {United States},
year = {2018},
month = {1}
}

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