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  • The Relationship between Molecular Structure and Foaming of Poly(ethylene glycol)—Poly(propylene glycol) Triblock Surfactants in Cementitious Materials
Title: The Relationship between Molecular Structure and Foaming of Poly(ethylene glycol)—Poly(propylene glycol) Triblock Surfactants in Cementitious Materials
Award ID(s):
1920127
PAR ID:
10534689
Author(s) / Creator(s):
;
Publisher / Repository:
MDPI
Date Published:
Journal Name:
Buildings
ISSN:
2075-5309
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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    This study investigates the relationship between the molecular structure and foaming of poly(ethylene glycol) and poly(propylene glycol) triblock copolymers in Portland cement pastes. Four copolymers with different molecular structures were studied at varying concentrations. All copolymers showed a reduction in surface tension of the cement pore solution; however, only some of them demonstrated foaming and air entraining in cement paste. The results indicated that the molecular structure parameter, hydrophilic-to-lipophilic balance (HLB), has a direct relationship with the foaming and air-entraining performance of the copolymers. The total organic carbon measurements showed very small adsorption of these non-ionic copolymers on hydrating cement particles due to the lack of surface charge needed to interact with the heterogeneously charged surface of hydrating cement. In addition, these copolymers did not seem to affect the flow of cement paste due to a lack of adsorption on cement particles. The cement paste modified with the copolymers showed increased water sorption compared to the control paste due to the increased capillary porosity and slight increase in pore surface hydrophilicity. However, the freeze-thaw resistance was shown to improve with an increase in the number of air voids in the modified cement pastes. The findings establish the relationship between molecular properties of copolymers and their air-entraining performance in cement paste to mitigate the damages caused by freeze-thaw action. 
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    Non-toxic, chemically inert, organic polymers as polyethylene glycol (PEG) and polyoxymethylene (POM) have versatile applications in basic research, industry and pharmacy. In this work, we aim to characterize the hydration structure of PEG and POM oligomers by exploring how the solute disturbs the water structure compared to the bulk solvent and how the solute chain interacts with the solvent. We explore the effect of (i) the C–C–O (PEG) versus C-O (POM) constitution of the chain and (ii) chain length. To this end, MD simulations followed by clustering and topological analysis of the hydration network, as well as quantum mechanical calculations of atomic charges are used. We show that the hydration varies with chain conformation and length. The degree of folding of the chain impacts its degree of solvation, which is measurable by different parameters as for example the number of water molecules in the first solvation shell and the solvent accessible surface. Atomic charges calculated on the oligomers in gas phase are stable throughout conformation and chain length and seem not to determine solvation. Hydration however induces charge transfer from the solute molecule to the solvent, which depends on the degree of hydration. 
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