Water Dynamics in Polyacrylamide Hydrogels
Abstract
Polymeric hydrogels have wide applications including electrophoresis, biocompatible materials, water superadsorbents, and contact lenses. The properties of hydrogels involve the poorly characterized molecular dynamics of water and solutes trapped within the three-dimensional cross-linked polymer networks. Here we apply ultrafast infrared two-dimensional infrared (2D IR) vibrational echo and polarization-selective pump-probe (PSPP) spectroscopies to investigate the ultrafast molecular dynamics of water and a small molecular anion solute, selenocyanate (SeCN-), in polyacrylamide hydrogels. For all mass concentrations of polymer studied (5% and above), the hydrogen bonding network reorganization (spectral diffusion) dynamics and reorientation dynamics reported by both water and SeCN- solvated by water are significantly slower than in bulk water. As the polymer mass concentration increases, molecular dynamics in the hydrogels slow further. The magnitudes of the slowing, measured with both water and SeCN-, are similar. However, the entire hydrogen bonding network of water molecules appear to slow down as a single ensemble, without a difference between the core water population and the interface water population at the polymer-water surface. In contrast, the dissolved SeCN- do exhibit two-component dynamics, where the major component is assigned to the anions fully solvated in the confined water nanopools. The slower component has a small amplitude whichmore »
- Authors:
-
- Stanford Univ., CA (United States). Department of Chemistry
- Publication Date:
- Research Org.:
- Stanford Univ., CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1485138
- Alternate Identifier(s):
- OSTI ID: 1788262
- Grant/Contract Number:
- FG03-84ER13251; FG02-84ER13251
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 140; Journal Issue: 30; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; hydrogels; dynamics; ultrafast infrared experiments; water dynamics in nanoconfinement; 36 MATERIALS SCIENCE; 14 SOLAR ENERGY
Citation Formats
Yan, Chang, Kramer, Patrick L., Yuan, Rongfeng, and Fayer, Michael D. Water Dynamics in Polyacrylamide Hydrogels. United States: N. p., 2018.
Web. doi:10.1021/jacs.8b03547.
Yan, Chang, Kramer, Patrick L., Yuan, Rongfeng, & Fayer, Michael D. Water Dynamics in Polyacrylamide Hydrogels. United States. https://doi.org/10.1021/jacs.8b03547
Yan, Chang, Kramer, Patrick L., Yuan, Rongfeng, and Fayer, Michael D. Mon .
"Water Dynamics in Polyacrylamide Hydrogels". United States. https://doi.org/10.1021/jacs.8b03547. https://www.osti.gov/servlets/purl/1485138.
@article{osti_1485138,
title = {Water Dynamics in Polyacrylamide Hydrogels},
author = {Yan, Chang and Kramer, Patrick L. and Yuan, Rongfeng and Fayer, Michael D.},
abstractNote = {Polymeric hydrogels have wide applications including electrophoresis, biocompatible materials, water superadsorbents, and contact lenses. The properties of hydrogels involve the poorly characterized molecular dynamics of water and solutes trapped within the three-dimensional cross-linked polymer networks. Here we apply ultrafast infrared two-dimensional infrared (2D IR) vibrational echo and polarization-selective pump-probe (PSPP) spectroscopies to investigate the ultrafast molecular dynamics of water and a small molecular anion solute, selenocyanate (SeCN-), in polyacrylamide hydrogels. For all mass concentrations of polymer studied (5% and above), the hydrogen bonding network reorganization (spectral diffusion) dynamics and reorientation dynamics reported by both water and SeCN- solvated by water are significantly slower than in bulk water. As the polymer mass concentration increases, molecular dynamics in the hydrogels slow further. The magnitudes of the slowing, measured with both water and SeCN-, are similar. However, the entire hydrogen bonding network of water molecules appear to slow down as a single ensemble, without a difference between the core water population and the interface water population at the polymer-water surface. In contrast, the dissolved SeCN- do exhibit two-component dynamics, where the major component is assigned to the anions fully solvated in the confined water nanopools. The slower component has a small amplitude which is correlated with the polymer mass concentration, and is assigned to adsorbed anions strongly interacting with the polymer fiber networks.},
doi = {10.1021/jacs.8b03547},
journal = {Journal of the American Chemical Society},
number = 30,
volume = 140,
place = {United States},
year = {Mon Jul 09 00:00:00 EDT 2018},
month = {Mon Jul 09 00:00:00 EDT 2018}
}
Web of Science
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