Antiplasticization and phase behavior in phase-separated modified starch-sucrose blends: A positron lifetime and solid-state NMR study

Francesca Martini, David J. Hughes, Gabriela Badolato Bönisch, Thomas Zwick, Christian Schäfer, Marco Geppi, M. Ashraf Alam, Job Ubbink

Research output: Contribution to journalArticlepeer-review

13 Scopus citations

Abstract

Interactions, organization and dynamics within phase-separated ternary blends of hydrophobically modified starch (HMS), sucrose and water are investigated using solid-state NMR and positron annihilation lifetime spectroscopy (PALS). Antiplasticization of HMS by sucrose is demonstrated by PALS and 1H NMR T1 measurements. Selective solid-state 13C NMR experiments show that a large fraction of sucrose is in molecular contact with HMS even at high sucrose contents, indicating that the HMS-sucrose phase separation is only partial. Sucrose is observed to migrate away from the HMS-rich domains at temperatures that are above the lower Tg, but still below the upper Tg. 1H spin diffusion experiments indicate that phase separation occurs on a nanometric scale, in line with recent theory (Van der Sman, Food Hydrocolloids 87, 360–370 (2019)). We infer that the nanoscale structure of the HMS-rich phase allows for intimate molecular contact between the HMS-rich and the sucrose-rich phases and explains the unusual dynamic behavior.

Original languageEnglish (US)
Article number116931
JournalCarbohydrate Polymers
Volume250
DOIs
StatePublished - Dec 15 2020

Bibliographical note

Funding Information:
We thank Giacomo Mencarini (Università di Pisa) for his contribution to carrying out the NMR experiments. We acknowledge financial support from EPSRC (Ref: EP/J500379/1 ).

Funding Information:
We thank Giacomo Mencarini (Universit? di Pisa) for his contribution to carrying out the NMR experiments. We acknowledge financial support from EPSRC (Ref: EP/J500379/1).

Publisher Copyright:
© 2020 Elsevier Ltd

Keywords

  • Amorphous phase separation
  • Antiplasticization
  • C CP-MAS
  • Free volume
  • H relaxation times
  • OSA-starch
  • Plasticization
  • Positron annihilation
  • Sucrose

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