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Title: Alternating crystalline lamellar structures from thermodynamically miscible poly(ε-caprolactone) H/D blends

Abstract

Thermodynamic interaction and non-isothermal crystallization behavior in a series of protiated (H-) and deuterated (D-) poly(ε-caprolactone) (PCL) blends have been systematically investigated. The blends were thermodynamically miscible in the melt. The Flory–Huggins interaction parameter (χ) between H- and D-PCL segments was estimated. The hydroxyl groups in the PCL chain-ends were found to contribute significantly to the negative χ values. Combined characterization of small-angle X-ray scattering (SAXS) and small-angle neutron scattering (SANS) revealed that upon slow cooling, unique alternating H-rich and D-rich PCL lamellar structures are formed regardless of the blend ratio, which is attributed to the Tc difference between H- and D-PCLs. While upon rapid cooling, mixed crystals of H- and D-PCLs are predominantly formed. These results provide insightful information on the melt thermodynamics as well as detailed chain arrangements in lamellar crystals for semi-crystalline H/D polyester blends.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [4];  [5];  [6]; ORCiD logo [2];  [7]; ORCiD logo [8];  [3]
  1. South China Univ. of Technology (SCUT), Guangzhou (China); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS); Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS); Univ. of Tennessee, Knoxville, TN (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS), and Neutron Scattering Division
  6. Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  7. South China Univ. of Technology (SCUT), Guangzhou (China)
  8. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1530188
Alternate Identifier(s):
OSTI ID: 1550762
Grant/Contract Number:  
AC02-06CH11357; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Polymer
Additional Journal Information:
Journal Volume: 175; Journal Issue: C; Journal ID: ISSN 0032-3861
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Co-crystallization; Deuterated poly(epsilon-caprolactone); Small-angle neutron scattering

Citation Formats

Li, Lengwan, Arras, Matthias M. L., Li, Tianyu, Li, Wei, Chang, Dongsook, Keum, Jong K., Bonnesen, Peter V., Qian, Shuo, Peng, Xiangfang, Lee, Byeongdu, and Hong, Kunlun. Alternating crystalline lamellar structures from thermodynamically miscible poly(ε-caprolactone) H/D blends. United States: N. p., 2019. Web. doi:10.1016/j.polymer.2019.05.055.
Li, Lengwan, Arras, Matthias M. L., Li, Tianyu, Li, Wei, Chang, Dongsook, Keum, Jong K., Bonnesen, Peter V., Qian, Shuo, Peng, Xiangfang, Lee, Byeongdu, & Hong, Kunlun. Alternating crystalline lamellar structures from thermodynamically miscible poly(ε-caprolactone) H/D blends. United States. doi:10.1016/j.polymer.2019.05.055.
Li, Lengwan, Arras, Matthias M. L., Li, Tianyu, Li, Wei, Chang, Dongsook, Keum, Jong K., Bonnesen, Peter V., Qian, Shuo, Peng, Xiangfang, Lee, Byeongdu, and Hong, Kunlun. Tue . "Alternating crystalline lamellar structures from thermodynamically miscible poly(ε-caprolactone) H/D blends". United States. doi:10.1016/j.polymer.2019.05.055. https://www.osti.gov/servlets/purl/1530188.
@article{osti_1530188,
title = {Alternating crystalline lamellar structures from thermodynamically miscible poly(ε-caprolactone) H/D blends},
author = {Li, Lengwan and Arras, Matthias M. L. and Li, Tianyu and Li, Wei and Chang, Dongsook and Keum, Jong K. and Bonnesen, Peter V. and Qian, Shuo and Peng, Xiangfang and Lee, Byeongdu and Hong, Kunlun},
abstractNote = {Thermodynamic interaction and non-isothermal crystallization behavior in a series of protiated (H-) and deuterated (D-) poly(ε-caprolactone) (PCL) blends have been systematically investigated. The blends were thermodynamically miscible in the melt. The Flory–Huggins interaction parameter (χ) between H- and D-PCL segments was estimated. The hydroxyl groups in the PCL chain-ends were found to contribute significantly to the negative χ values. Combined characterization of small-angle X-ray scattering (SAXS) and small-angle neutron scattering (SANS) revealed that upon slow cooling, unique alternating H-rich and D-rich PCL lamellar structures are formed regardless of the blend ratio, which is attributed to the Tc difference between H- and D-PCLs. While upon rapid cooling, mixed crystals of H- and D-PCLs are predominantly formed. These results provide insightful information on the melt thermodynamics as well as detailed chain arrangements in lamellar crystals for semi-crystalline H/D polyester blends.},
doi = {10.1016/j.polymer.2019.05.055},
journal = {Polymer},
number = C,
volume = 175,
place = {United States},
year = {2019},
month = {5}
}

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