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Title: Reversible Self-Assembly of Glutathione-Coated Gold Nanoparticle Clusters via pH-Tunable Interactions

Abstract

In this study, nanoparticle (NP) clusters with diameters ranging from 20 to 100 nm are reversibly assembled from 5 nm gold (Au) primary particles coated with glutathione (GSH) in aqueous solution as a function of pH in the range of 5.4 to 3.8. As the pH is lowered, the GSH surface ligands become partially zwitterionic and form interparticle hydrogen bonds that drive the self-limited assembly of metastable clusters in <1 min. Whereas clusters up to 20 nm in size are stable against cluster–cluster aggregation for up to 1 day, clusters up to 80 nm in size can be stabilized over this period via the addition of citrate to the solution in equal molarity with GSH molecules. The cluster diameter may be cycled reversibly by tuning pH to manipulate the colloidal interactions; however, modest background cluster–cluster aggregation occurs during cycling. Cluster sizes can be stabilized for at least 1 month via the addition of PEG-thiol as a grafted steric stabilizer, where PEG-grafted clusters dissociate back to starting primary NPs at pH 7 in fewer than 3 days. Whereas the presence of excess citrate has little effect on the initial size of the metastable clusters, it is necessary for both the cyclingmore » and dissociation to mediate the GSH–GSH hydrogen bonds. In conclusion, these metastable clusters exhibit significant characteristics of equilibrium self-limited assembly between primary particles and clusters on time scales where cluster–cluster aggregation is not present.« less

Authors:
 [1];  [2];  [3];  [1];  [1]; ORCiD logo [4]; ORCiD logo [1]
  1. Univ. of Texas, Austin, TX (United States). McKetta Department of Chemical Engineering
  2. Univ. of Texas, Austin, TX (United States). McKetta Department of Chemical Engineering; Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies
  3. Univ. of Texas, Austin, TX (United States). Texas Materials Institute
  4. Univ. of Texas, Austin, TX (United States). McKetta Department of Chemical Engineering and Texas Materials Institute
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1441463
Report Number(s):
SAND-2018-4149J
Journal ID: ISSN 0743-7463; 662768
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Langmuir
Additional Journal Information:
Journal Volume: 33; Journal Issue: 43; Journal ID: ISSN 0743-7463
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Moaseri, Ehsan, Bollinger, Jonathan A., Changalvaie, Behzad, Johnson, Lindsay, Schroer, Joseph, Johnston, Keith P., and Truskett, Thomas M. Reversible Self-Assembly of Glutathione-Coated Gold Nanoparticle Clusters via pH-Tunable Interactions. United States: N. p., 2017. Web. doi:10.1021/acs.langmuir.7b02446.
Moaseri, Ehsan, Bollinger, Jonathan A., Changalvaie, Behzad, Johnson, Lindsay, Schroer, Joseph, Johnston, Keith P., & Truskett, Thomas M. Reversible Self-Assembly of Glutathione-Coated Gold Nanoparticle Clusters via pH-Tunable Interactions. United States. doi:10.1021/acs.langmuir.7b02446.
Moaseri, Ehsan, Bollinger, Jonathan A., Changalvaie, Behzad, Johnson, Lindsay, Schroer, Joseph, Johnston, Keith P., and Truskett, Thomas M. Fri . "Reversible Self-Assembly of Glutathione-Coated Gold Nanoparticle Clusters via pH-Tunable Interactions". United States. doi:10.1021/acs.langmuir.7b02446. https://www.osti.gov/servlets/purl/1441463.
@article{osti_1441463,
title = {Reversible Self-Assembly of Glutathione-Coated Gold Nanoparticle Clusters via pH-Tunable Interactions},
author = {Moaseri, Ehsan and Bollinger, Jonathan A. and Changalvaie, Behzad and Johnson, Lindsay and Schroer, Joseph and Johnston, Keith P. and Truskett, Thomas M.},
abstractNote = {In this study, nanoparticle (NP) clusters with diameters ranging from 20 to 100 nm are reversibly assembled from 5 nm gold (Au) primary particles coated with glutathione (GSH) in aqueous solution as a function of pH in the range of 5.4 to 3.8. As the pH is lowered, the GSH surface ligands become partially zwitterionic and form interparticle hydrogen bonds that drive the self-limited assembly of metastable clusters in <1 min. Whereas clusters up to 20 nm in size are stable against cluster–cluster aggregation for up to 1 day, clusters up to 80 nm in size can be stabilized over this period via the addition of citrate to the solution in equal molarity with GSH molecules. The cluster diameter may be cycled reversibly by tuning pH to manipulate the colloidal interactions; however, modest background cluster–cluster aggregation occurs during cycling. Cluster sizes can be stabilized for at least 1 month via the addition of PEG-thiol as a grafted steric stabilizer, where PEG-grafted clusters dissociate back to starting primary NPs at pH 7 in fewer than 3 days. Whereas the presence of excess citrate has little effect on the initial size of the metastable clusters, it is necessary for both the cycling and dissociation to mediate the GSH–GSH hydrogen bonds. In conclusion, these metastable clusters exhibit significant characteristics of equilibrium self-limited assembly between primary particles and clusters on time scales where cluster–cluster aggregation is not present.},
doi = {10.1021/acs.langmuir.7b02446},
journal = {Langmuir},
number = 43,
volume = 33,
place = {United States},
year = {2017},
month = {10}
}

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