Interfacial Properties of Polymer Nanocomposites: Role of Chain Rigidity and Dynamic Heterogeneity Length Scale

Cheng, Shiwang; Carroll, Bobby; Lu, Wei; Fan, Fei; Carrillo, Jan-Michael Y.; Martin, Halie; Holt, Adam P.; Kang, Nam-Goo; Bocharova, Vera; Mays, Jimmy W.; Sumpter, Bobby G.; Dadmun, Mark; Sokolov, Alexei P.

doi:10.1021/acs.macromol.6b02816

Interfacial Properties of Polymer Nanocomposites: Role of Chain Rigidity and Dynamic Heterogeneity Length Scale

Journal Article · Wed Mar 15 00:00:00 EDT 2017 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.6b02816· OSTI ID:1376457

^[1]; Carroll, Bobby ^[2]; ^[2]; ^[2]; ^[3]; Martin, Halie ^[2]; ^[2]; ^[4]; Bocharova, Vera ^[1]; Mays, Jimmy W. ^[4]; ^[3]; ^[4]; Sokolov, Alexei P. ^[4]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

While it is known that the properties of polymer nanocomposites are largely dominated by the interfacial layer around nanoparticles, the molecular parameters controlling the interfacial layer structure and dynamics remain unknown. In this paper we combine small-angle X-ray scattering, differential scanning calorimetry, and broadband dielectric spectroscopy to analyze the dependence of the interfacial layer thickness, l_int, on polymer rigidity defined through the characteristic ratio, C_∞. This analysis revealed a value of C_∞ ~ 5–7, beyond which l_int increases substantially with C_∞. Moreover, l_int grows upon approaching the glass transition temperature from above, and the rate of this growth seems to correlate with polymer fragility. Most important, our analysis revealed that l_int is comparable to the characteristic length scale of dynamic heterogeneities in the studied materials. Finally, these results provide new understandings of molecular parameters controlling the interfacial layer and are important not only for the field of polymer nanocomposites but also for the fields of thin polymer films and dynamics of soft matter in general.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1376457

Journal Information:: Macromolecules, Journal Name: Macromolecules Journal Issue: 6 Vol. 50; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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