Quantitative Determination of Metal Ion Adsorption on Cellulose Nanocrystals Surfaces

Harrison R. Paul, Mrinal K. Bera, Nicholas Macke, Stuart J. Rowan, Matthew V. Tirrell

Research output: Contribution to journalArticlepeer-review

Abstract

Nanocellulose is a bio-based material that holds significant potential in the field of water purification. Of particular interest is their potential use as a key sorbent material for the removal of metal ions from solution. However, the structure of metal ions adsorbed onto cellulose surfaces is not well understood. The focus of this work is to determine quantitatively the three-dimensional distribution of metal ions of different valencies surrounding negatively charged carboxylate functionalized cellulose nanocrystals (CNCs) using anomalous small-angle X-ray scattering (ASAXS). These distributions can affect the water and ionic permeability in these materials. The data show that increasing the carboxylate density on the surface of the CNCs from 740 to 1100 mmol/kg changed the nature of the structure of the adsorbed ions from a monolayer into a multilayer structure. The monolayer was modeled as a Stern layer around the CNC nanoparticles, whereas the multilayer structure was modeled as a diffuse layer on top of the Stern layer around the nanoparticles. Within the Stern layer, the maximum ion density increases from 1680 to 4350 mmol of Rb+/(kg of CNC) with the increase in the carboxylate density on the surface of the nanoparticles. Additionally, the data show that CNCs can leverage multiple mechanisms, such as electrostatic attraction and the chaotropic effect, to adsorb ions of different valencies. By understanding the spatial organization of the adsorbed metal ions, the design of cellulose-based sorbents can be further optimized to improve the uptake capacity and selectivity in separation applications.

Original languageEnglish (US)
Pages (from-to)1921-1930
Number of pages10
JournalACS nano
Volume18
Issue number3
DOIs
StatePublished - Jan 23 2024
Externally publishedYes

Bibliographical note

Publisher Copyright:
© 2024 The Authors. Published by American Chemical Society

Keywords

  • Adsorption
  • Anomalous Small Angle X-ray Scattering
  • Cellulose Nanocrystals
  • Ion Exchange
  • Sorbents
  • Water Purification

PubMed: MeSH publication types

  • Journal Article

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