, Volume 26, Issue 3, pp 1449–1466 | Cite as

A molecular dynamics model to measure forces between cellulose fibril surfaces: on the effect of non-covalent polyelectrolyte adsorption

  • Carlos Sáenz EzquerroEmail author
  • Cristina Crespo Miñana
  • Salvador Izquierdo
  • Manuel Laspalas
Original Research


This study describes the development of representative models of cellulose fibril surface (CFS) as a first approximation to the study of the molecular interactions that are developed between cellulose fibres. In order to assess its sensitivity and representativeness towards the main factors affecting the bonding properties at the fibre scale, these models were non-covalently surface modified with two types of polyelectrolytes, sodium carboxymethyl cellulose (CMC–ONa) and a cationic polyacrylamide (CPAM). From the analysis of pair correlation functions (g(r)) it was possible to assess the main interactions of adsorption of polyelectrolytes towards the (1–10) hydrophilic cellulose, which were due to electrostatic interactions coupled with hydrogen bonding. Besides, the bond strength between fibril surfaces through the (100) hydrophobic surface was calculated from pull out simulations (using steered molecular dynamics). Using a rate of change of force of 0.159 nN ps−1, the calculated bond strength for the neat CFS model (nanometer scale) was two to three orders of magnitude higher than the experimental values observed at the fibre scale (micrometer scale). The results for the polyelectrolyte modified setups supported the validity of the CFS models to reproduce the expected behavior of inter-fibre joints in terms of the specific bond strength and the relative bonded area at the fibre scale in cellulose materials, and thereby the CFS models are a suitable complement, in conjunction with other techniques, for the systematic study of the effect (in qualitative terms) of chemical or physical factors on the bond strength properties of cellulosic materials.

Graphical abstract


Molecular dynamics Bond strength Force Polyelectrolyte Adsorption Pull out 



This work has been partly granted by Spanish Ministry of Economy, Industry and Competitiveness (project RTC-2014-2817-5) and by FSE Operative Programme for Aragon (2014-2020).

Supplementary material

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Supplementary material 1 (PDF 9019 kb)
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Supplementary material 2 (PDF 1016 kb)
10570_2018_2166_MOESM3_ESM.pdf (571 kb)
Supplementary material 3 (PDF 571 kb)


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Copyright information

© Springer Nature B.V. 2018

Authors and Affiliations

  1. 1.Aragon Institute of Technology ITAINNOVASaragossaSpain

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