Contact and macroscopic ageing in colloidal suspensions

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Abstract

The ageing behaviour of dense suspensions or pastes at rest is almost exclusively attributed to structural dynamics. Here, we identify another ageing process, contact-controlled ageing, consisting of the progressive stiffening of solid–solid contacts of an arrested colloidal suspension. By combining rheometry, confocal microscopy and particle-scale mechanical tests using laser tweezers, we demonstrate that this process governs the shear-modulus ageing of dense aqueous silica and polymer latex suspensions at moderate ionic strengths. We further show that contact-controlled ageing becomes relevant as soon as Coulombic interactions are sufficiently screened out that the formation of solid–solid contacts is not limited by activation barriers. Given that this condition only requires moderate ion concentrations, contact-controlled ageing should be generic in a wide class of materials, such as cements, soils or three-dimensional inks, thus questioning our understanding of ageing dynamics in these systems.

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Fig. 1: Mechanical ageing in dense silica suspensions.
Fig. 2: Absence of structural ageing in a water–glycerol mixture.
Fig. 3: Laser-tweezer bending test.
Fig. 4: Matching microscopic and macroscopic data.
Fig. 5: Macroscopic and contact ageing in PMMA suspensions.

Data availability

Figure source data are provided online; other data used in this work are available from the authors.

Code availability

The software used in this work is available from the authors.

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Acknowledgements

This work benefited from a French government grant managed by ANR within the framework of the National Program Investments for the Future, ANR-11-LABX-0022-01. F.B.’s stay at the University of Delaware was supported by University Paris-Est.

Author information

X.C., J.G. and A.L. conceived and supervised the project. J.G. and J.F. designed the macroscopic shear-modulus ageing protocol and obtained data on silica suspensions. J.G. supervised sample preparation and all experiments. E.M.F. designed the laser tweezer three-point flexural test and supervised its use. F.B. obtained complementary macroscopic shear modulus data, designed the two-compartment cell, performed flexural ageing measurements with E.M.F. and J.G. All authors contributed to the interpretation of experimental data, model construction and article planning and writing.

Correspondence to Xavier Chateau or Anaël Lemaître.

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Supplementary information

41563_2020_624_MOESM2_ESM.avi

Two videos running in parallel show the contact formation and opening tests at two ionic strengths.

Supplementary Information

Supplementary Video, Notes 1 and 2, Methods, Figs. 1–5 and References.

Supplementary Video 1

Two videos running in parallel show the contact formation and opening tests at two ionic strengths.

Source data

Source Data Fig. 1

Shear modulus versus ageing time data.

Source Data Fig. 2

Unprocessed confocal images at ageing times t = 1, 5 and 10 min.

Source Data Fig. 3

Source data. Page 1, force versus deflection data at three ageing times and pages 2–4, deduced bond rigidity for three ionic strengths and two rod sizes.

Source Data Fig. 4

Source data. Page 1, shear modulus versus bond rigidity and page 2, S versus packing fraction.

Source Data Fig. 5

Source data. Pages 1–4, bond rigidity versus time. Pages 5 and 6, shear-modulus ageing. Page 7, shear modulus versus bond rigidity.

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Bonacci, F., Chateau, X., Furst, E.M. et al. Contact and macroscopic ageing in colloidal suspensions. Nat. Mater. (2020). https://doi.org/10.1038/s41563-020-0624-9

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