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Fig 1.

Frequency sweep curve of 2 wt% OCNF samples.

OCNF (2 wt%) with either 1 wt% Laponite (orange squares) or 1 wt% montmorillonite (blue circles).

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Fig 1 Expand

Fig 2.

The tan(δ) values of mixtures of Laponite and montmorillonite with OCNF.

The negative error bars of 0.5 and 1 wt% montmorillonite in 0.75 wt% OCNF go beyond zero and are therefore not displayed on a log plot.

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Fig 2 Expand

Fig 3.

Flow sweeps of OCNF and clays.

Flow sweep curves of 2 wt% OCNF (blue crosses), 1.5 wt% OCNF (blue circles), and 1.5 wt% OCNF with 0.5 wt% of either Laponite (green squares) or montmorillonite (orange triangles).

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Fig 3 Expand

Fig 4.

Amplitude sweep curves of 1 wt% Laponite (orange squares) and 1 wt% montmorillonite (blue circles) in 1.5 wt% OCNF.

Storage moduli (G’) shown with filled symbols, loss moduli (G") shown in open symbols.

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Fig 4 Expand

Fig 5.

Yield strains (top) and yield stresses (bottom) of mixtures of Laponite and montmorillonite with OCNF, taken from the amplitude sweep curves (see Supporting information).

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Fig 5 Expand

Fig 6.

SAXS scattering data from OCNF and clay dispersions.

A) 1.5 wt% OCNF, 1 wt% Laponite in water, and 1 wt% Laponite in 1.5 wt% OCNF. The black line is the scattering of 1.5 wt% OCNF and 1 wt% Laponite in water added together. B) 1.5 wt% OCNF, 1 wt% montmorillonite in water, and 1 wt% Laponite in 1.5 wt% OCNF. The black line is the scattering of 1.5 wt% OCNF and 1 wt% montmorillonite in water added together, with normalization for intensity.

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Fig 6 Expand

Fig 7.

Graphical illustration of the cellulose fibril and clay interactions.

Laponite (A) and montmorillonite (B) clay particles interact with the cellulose nanofibrils (green). Aggregates of the smaller laponite particles are more able to fit into and interact with the OCNF network than the much large aggregates of montmorillonite which leads to stronger interactions and more ‘gel-like’ properties.

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Fig 7 Expand