Surface Charge Influence on the Phase Separation and Viscosity of Cellulose Nanocrystals

Tiffany Abitbol, Doron Kam, Yael Levi-Kalisman, Derek G. Gray, Oded Shoseyov

Research output: Contribution to journalArticlepeer-review

Abstract

A series of four cellulose nanocrystal (CNC) suspensions were prepared from bleached softwood kraft pulp using different conditions of sulfuric acid hydrolysis. The CNCs were identical in size (95 nm in length × 5 nm in width) but had different surface charges corresponding to the harshness of the hydrolysis conditions. Consequently, it was possible to isolate the effects of surface charge on the self-assembly and viscosity of the CNC suspensions across surface charges ranging from 0.27%S to 0.89%S. The four suspensions (never-dried, free of added electrolyte) all underwent liquid crystalline phase separation, but the concentration onset for the emergence of the chiral nematic phase shifted to higher values with increasing surface charge. Similarly, suspension viscosity was also influenced by surface charge, with suspensions of lower surface charge CNCs more viscous and tending to gel at lower concentrations. The properties of the suspensions were interpreted in terms of the increase in effective diameter of the nanocrystals due to the surface electrostatic repulsion of the negative sulfate half-esters, as modified by the screening effects of the H+ counterions in the suspensions. The results suggest that there is a threshold surface charge density (∼0.3%S) above which effective volume considerations are dominant across the concentration range relevant to liquid crystalline phase formation. Above this threshold value, phase separation occurs at the same effective volume fraction of CNCs (∼10 vol %), with a corresponding increase in critical concentration due to the decrease in effective diameter that occurs with increasing surface charge. Below or near this threshold value, the formation of end-to-end aggregates may favor gelation and interfere with ordered phase formation.

Original languageEnglish
Pages (from-to)3925-3933
Number of pages9
JournalLangmuir
Volume34
Issue number13
DOIs
StatePublished - 3 Apr 2018

All Science Journal Classification (ASJC) codes

  • Condensed Matter Physics
  • Spectroscopy
  • General Materials Science
  • Surfaces and Interfaces
  • Electrochemistry

Fingerprint

Dive into the research topics of 'Surface Charge Influence on the Phase Separation and Viscosity of Cellulose Nanocrystals'. Together they form a unique fingerprint.

Cite this