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

doi:10.1021/acsami.7b13309

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

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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:

Nguyen, Manh-Thuong ^[1]; Wang, Zheming ^[1];

^[1]; Childers, M. Ian ^[1];

^[1]; Koech, Phillip K. ^[1]; Bennett, Wendy D. ^[1];

^[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:: 2018-01-09

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

Journal Name:: ACS Applied Materials and Interfaces

Additional Journal Information:: Journal Volume: 10; Journal Issue: 3; Journal ID: ISSN 1944-8244

Publisher:: American Chemical Society (ACS)

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.

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                    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.

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                    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.

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@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},

  issn         = {1944-8244},

  number       = 3,

  volume       = 10,

  place        = {United States},

  year         = {2018},

  month        = {1}

}

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DOI: 10.1021/acsami.7b13309

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