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Title: Atomic Origins of the Self-Healing Function in Cement–Polymer Composites

Abstract

Motivated by recent advances in self-healing cement and epoxy polymer composites, we present a combined ab initio molecular dynamics and sum frequency generation (SFG) spectroscopy study of a calcium-silicate-hydrate/polymer interface. On stable, low-defect surfaces, the polymer only weakly adheres through coordination and hydrogen bonding interactions and can be easily mobilized towards defected surfaces. Conversely, on fractured surfaces, the polymer strongly anchors through ionic Ca-O bonds resulting from the deprotonation of polymer hydroxyl groups. In addition, polymer S-S groups are turned away from the cement/polymer interface, allowing for the self-healing function within the polymer. The overall elasticity and healing properties of these composites stem from a flexible hydrogen bonding network that can readily adapt to surface morphology. The theoretical vibrational signals associated with the proposed cement-polymer interfacial chemistry were confirmed experimentally by SFG spectroscopy.

Authors:
 [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Basic and Applied Molecular Foundations, Physical and Computational Sciences Directorate, ‡Energy and Environment Directorate, and §Geochemistry, Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, United States
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Geothermal Technologies Office (EE-4G)
OSTI Identifier:
1419916
Report Number(s):
PNNL-SA-130887
Journal ID: ISSN 1944-8244; 50121; GT0300000
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Applied Materials and Interfaces; Journal Volume: 10; Journal Issue: 3
Country of Publication:
United States
Language:
English
Subject:
Cement polymer composites; SFG; AIMD; self-healing; geothermal; cementitious materials; self-healing cement-polymer composites; ab initio molecular 8 dynamics; polymer - calcium silicate hydrate interactions; Environmental Molecular Sciences Laboratory

Citation Formats

Nguyen, Manh-Thuong, Wang, Zheming, Rod, Kenton A., Childers, M. Ian, Fernandez, Carlos, Koech, Phillip K., Bennett, Wendy D., Rousseau, Roger, and Glezakou, Vassiliki-Alexandra. Atomic Origins of the Self-Healing Function in Cement–Polymer Composites. United States: N. p., 2018. Web. doi:10.1021/acsami.7b13309.
Nguyen, Manh-Thuong, Wang, Zheming, Rod, Kenton A., Childers, M. Ian, Fernandez, Carlos, Koech, Phillip K., Bennett, Wendy D., Rousseau, Roger, & Glezakou, Vassiliki-Alexandra. Atomic Origins of the Self-Healing Function in Cement–Polymer Composites. United States. doi:10.1021/acsami.7b13309.
Nguyen, Manh-Thuong, Wang, Zheming, Rod, Kenton A., Childers, M. Ian, Fernandez, Carlos, Koech, Phillip K., Bennett, Wendy D., Rousseau, Roger, and Glezakou, Vassiliki-Alexandra. Tue . "Atomic Origins of the Self-Healing Function in Cement–Polymer Composites". United States. doi:10.1021/acsami.7b13309.
@article{osti_1419916,
title = {Atomic Origins of the Self-Healing Function in Cement–Polymer Composites},
author = {Nguyen, Manh-Thuong and Wang, Zheming and Rod, Kenton A. and Childers, M. Ian and Fernandez, Carlos and Koech, Phillip K. and Bennett, Wendy D. and Rousseau, Roger and Glezakou, Vassiliki-Alexandra},
abstractNote = {Motivated by recent advances in self-healing cement and epoxy polymer composites, we present a combined ab initio molecular dynamics and sum frequency generation (SFG) spectroscopy study of a calcium-silicate-hydrate/polymer interface. On stable, low-defect surfaces, the polymer only weakly adheres through coordination and hydrogen bonding interactions and can be easily mobilized towards defected surfaces. Conversely, on fractured surfaces, the polymer strongly anchors through ionic Ca-O bonds resulting from the deprotonation of polymer hydroxyl groups. In addition, polymer S-S groups are turned away from the cement/polymer interface, allowing for the self-healing function within the polymer. The overall elasticity and healing properties of these composites stem from a flexible hydrogen bonding network that can readily adapt to surface morphology. The theoretical vibrational signals associated with the proposed cement-polymer interfacial chemistry were confirmed experimentally by SFG spectroscopy.},
doi = {10.1021/acsami.7b13309},
journal = {ACS Applied Materials and Interfaces},
number = 3,
volume = 10,
place = {United States},
year = {Tue Jan 09 00:00:00 EST 2018},
month = {Tue Jan 09 00:00:00 EST 2018}
}