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1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions Tiago B. Becher, a Carolyne B. Braga, a Diego L. Bertuzzi, a Miguel D. Ramos Jr, a Ayaz Hassan, b Frank N. Crespilho, b Catia Ornelas a, * Table S1. Assignment of the vibrational modes observed in the FTIR spectra of Laponite, HN5, HNP5, HN5NaCl, HN5CaCl 2 , and HN5CeCl 3 . 0.1 1 10 100 1000 10 0 10 1 10 2 10 3 10 4 10 5 10 6 G' G'' G' and G'' (Pa) Strain (%) Figure S.I.1. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5. 0.1 1 10 100 10 0 10 1 10 2 10 3 10 4 10 5 10 6 G' G'' G' and G'' (Pa) f in Hz Compound -OH stretching of lattice hydroxyl group (cm -1 ) -OH stretching from free H 2 O (cm -1 ) H-OH bending (cm -1 ) Si-O streching (cm -1 ) Laponite 3630 3410 1635 960 HN5 3630 3310 1635 1000 HNP5 3630 3310 1635 1000 HN5NaCl 3630 3310 1635 1000 HN5CaCl 2 3630 3310 1635 1005 HN5CeCl 3 3630 3310 1635 1005 Electronic Supplementary Material (ESI) for Soft Matter. This journal is © The Royal Society of Chemistry 2018

SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

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Page 1: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

1

Supporting Information

Structure-Property Relationship in Laponite Materials: From Wigner Glasses to

Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

Tiago B. Becher,a Carolyne B. Braga,a Diego L. Bertuzzi,a Miguel D. Ramos Jr,a Ayaz Hassan,b Frank N.

Crespilho,b Catia Ornelasa,*

Table S1. Assignment of the vibrational modes observed in the FTIR spectra of Laponite, HN5, HNP5,

HN5NaCl, HN5CaCl2, and HN5CeCl3.

0.1 1 10 100 1000100

101

102

103

104

105

106

G' G''

Clay 5%

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.1. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5%

G' a

nd G

'' (P

a)

f in Hz

Compound -OH stretching of lattice hydroxyl group

(cm-1

)

-OH stretching from free H2O (cm-1)

H-OH bending (cm-1)

Si-O streching (cm-1)

Laponite 3630 3410 1635 960

HN5 3630 3310 1635 1000 HNP5 3630 3310 1635 1000 HN5NaCl 3630 3310 1635 1000 HN5CaCl

2 3630 3310 1635 1005

HN5CeCl3 3630 3310 1635 1005

Electronic Supplementary Material (ESI) for Soft Matter.This journal is © The Royal Society of Chemistry 2018

Page 2: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

2

0.1 1 10 100 1000100

101

102

103

104

105

106

G' G''

Clay 4%

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.2. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN4.

0.1 1 10 100 1000100

101

102

103

104

105

106

G' G''

Clay 3%

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.3. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN3.

0.1 1 10 100 1000100

101

102

103

104

105

106

G' G''

Clay 2%

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.4. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN2.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 4%

G' a

nd G

'' (P

a)

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 3%

G' a

nd G

'' (P

a)

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 2%

G' a

nd G

'' (P

a)

f in Hz

Page 3: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

3

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.5. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

C4% + Polymer 5 + PBS 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.6. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN4NaCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 3% + Polymer 5mg + PBS 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.7. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN3NaCl.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 4% + Polymer 5mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 3% + Polymer 5mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 4: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

4

Variation of polymer

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 1mg + PBS 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.8. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 1 mg of polyacrylate.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 2.5mg + PBS 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.9. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 2.5 mg of polyacrylate.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.10. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 5 mg of polyacrylate.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 1mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 2.5mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 5: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

5

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.11. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 10 mg of polyacrylate.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 15mg + PBS 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.12. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 15 mg of polyacrylate.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 20mg + PBS 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.13. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 20 mg of polyacrylate.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 10mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 15mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 20mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 6: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

6

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 25mg + PBS 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.14. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 25 mg of polyacrylate.

Variation of PBS

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.01 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.15. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5PBS, using 0.01 M PBS.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.02 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.16. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5PBS, using 0.02 M PBS.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 25mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.01 M

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + PBS 0.02 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 7: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

7

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.03 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.17. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5PBS, using 0.03 M PBS.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.04 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.18. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5PBS, using 0.04 M PBS.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.05 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.19. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5PBS, using 0.05 M PBS.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + PBS 0.03 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.04 mL

G' G''

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.05 mL

G' G''

G' i

n Pa

G''

in P

a

f in Hz

Page 8: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

8

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.20. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5PBS, using 0.1 M PBS.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.2 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.21. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5PBS, using 0.2 M PBS.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.3 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.22. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5PBS, using 0.3 M PBS.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + PBS 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

G' i

n Pa

G''

in P

a

Clay 5% + Polymer 5mg + PBS 0.2 mL

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + PBS 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 9: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

9

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + PBS 0.4 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.23. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5PBS, using 0.4 M PBS.

Variation of NaCl

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaCl 0.01 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.24. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 0.01 M NaCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaCl 0.03 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.25. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 0.03 M NaCl.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + PBS 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.01 M NaCl

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + NaCl 0.03 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 10: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

10

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaCl 0.04 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.26. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 0.04 M NaCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaCl 0.05 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.27. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 0.05 M NaCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaCl 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.28. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 0.1 M NaCl.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaCl 0.04 mL

G' G''

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + NaCl 0.05 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + NaCl 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 11: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

11

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaCl 0.2 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.29. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 0.2 M NaCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaCl 0.3 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.30. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 0.3 M NaCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaCl 0.04 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.31. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaCl, using 0.4 M NaCl.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + NaCl 0.2 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + NaCl 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + NaCl 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 12: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

12

Variation of Na2SO4

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaSO4 0.01 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.32. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Na2SO4, using 0.01 M Na2SO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.03 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.33. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Na2SO4, using 0.03 M Na2SO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.04 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.34. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Na2SO4, using 0.04 M Na2SO4.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.01 M

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Na2SO4 0.03 mLG

' in

Pa G

'' in

Pa

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Na2SO4 0.04 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 13: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

13

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.05mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.35. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Na2SO4, using 0.05 M Na2SO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.36. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Na2SO4, using 0.1 M Na2SO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.2mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.37. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Na2SO4, using 0.2 M Na2SO4.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Na2SO4 0.05 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.1 mL

G' G''

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Na2SO4 0.2 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 14: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

14

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.3mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.38. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Na2SO4, using 0.3 M Na2SO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.4mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.39. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Na2SO4, using 0.4 M Na2SO4.

Variation of NaI

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaI 0.01 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.40. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaI, using 0.01 M NaI.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Na2SO4 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaI 0.01 M

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 15: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

15

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaI 0.03 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.41. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaI, using 0.03 M NaI.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaI 0.04 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.42. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaI, using 0.04 M NaI.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaI 0.05 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.43. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaI, using 0.05 M NaI.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Nal 0.03 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Nal 0.04 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Nal 0.05 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 16: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

16

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaI 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.44. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaI, using 0.1 M NaI.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaI 0.2 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.45. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaI, using 0.2 M NaI.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaI 0.3 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.46. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaI, using 0.3 M NaI.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Nal 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Nal 0.2 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Nal 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 17: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

17

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + NaI 0.4 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.47. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5NaI, using 0.4 M NaI.

Variation of MgSO4

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.01mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.48. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5MgSO4, using 0.01 M MgSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.03mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.49. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5MgSO4, using 0.03 M MgSO4.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Nal 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.01 M

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + MgSO4 0.03 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 18: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

18

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.04mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.50. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5MgSO4, using 0.04 M MgSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.05mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.51. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5MgSO4, using 0.05 M MgSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.52. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5MgSO4, using 0.1 M MgSO4.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + MgSO4 0.04 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.05 mL

G' G''

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + MgSO4 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 19: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

19

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.2mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.53. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5MgSO4, using 0.2 M MgSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.3mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.54. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5MgSO4, using 0.3 M MgSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.4mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.55. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5MgSO4, using 0.4 M MgSO4.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + MgSO4 0.2 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + MgSO4 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 20: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

20

Variation of CaCl2

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CaCl2 0.01mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.56. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CaCl2, using 0.01 M CaCl2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CaCl2 0.03 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.57. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CaCl2, using 0.03 M CaCl2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CaCl2 0.04 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.58. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CaCl2, using 0.04 M CaCl2.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CaCl2 0.01 M

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + CaCl2 0.03 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + CaCl2 0.04 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 21: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

21

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CaCl2 0.05 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.59. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CaCl2, using 0.05 M CaCl2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CaCl2 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.60. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CaCl2, using 0.1 M CaCl2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CaCl2 0.2 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.61. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CaCl2, using 0.2 M CaCl2.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + CaCl2 0.05 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + CaCl2 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + CaCl2 0.2 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 22: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

22

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CaCl2 0.3mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.62. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CaCl2, using 0.3 M CaCl2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CaCl2 0.3 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.63. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CaCl2, using 0.4 M CaCl2.

Variation of CuSO4

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.01mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.64. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CuSO4, using 0.01 M CuSO4.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + CaCl2 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + CaCl2 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.01 M

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 23: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

23

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.03 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.65. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CuSO4, using 0.03 M CuSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.04 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.66. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CuSO4, using 0.04 M CuSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.05 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.67. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CuSO4, using 0.05 M CuSO4.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.03 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.04 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.05 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 24: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

24

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.68. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CuSO4, using 0.1 M CuSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.69. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CuSO4, using 0.2 M CuSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.3 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.70. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CuSO4, using 0.3 M CuSO4.

0.1 1 10 100101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.2 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 25: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

25

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.04 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.71. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CuSO4, using 0.4 M CuSO4.

Variation of CeCl3

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.01mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.72. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CeCl3, using 0.01 M CeCl3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.03 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.73. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CeCl3, using 0.03 M CeCl3.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CuSO4 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.01 M

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.03 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 26: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

26

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.04 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.74. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CeCl3, using 0.04 M CeCl3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.05 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.75. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CeCl3, using 0.05 M CeCl3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.1 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.76. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CeCl3, using 0.1 M CeCl3.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.04 mL CeCl3

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.05 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 27: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

27

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.2 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.77. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CeCl3, using 0.2 M CeCl3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.3 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.78. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CeCl3, using 0.3 M CeCl3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.4 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.79. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5CeCl3, using 0.4 M CeCl3.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.2 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + CeCl3 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 28: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

28

Variation of KCl

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KCl 0.01mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.80. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KCl, using 0.01 M KCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KCl 0.03mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.81. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KCl, using 0.03 M KCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KCl 0.04mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.82. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KCl, using 0.04 M KCl.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KCl 0.01 M

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + KCl 0.03 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + KCl 0.04 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 29: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

29

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KCl 0.05mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.83. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KCl, using 0.05 M KCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KCl 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.84. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KCl, using 0.1 M KCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KCl 0.2mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.85. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KCl, using 0.2 M KCl.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + KCl 0.05 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + KCl 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + KCl 0.2 mL

G' i

n Pa

G''

in P

a

f in Hz

Page 30: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

30

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KCl 0.3mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.86. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KCl, using 0.3 M KCl.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KCl 0.4mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.87. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KCl, using 0.4 M KCl.

Variation of KNO3

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.01mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.88. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KNO3, using 0.01 M KNO3.

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + KCl 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + KCl 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.01 M

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 31: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

31

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.03mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.89. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KNO3, using 0.03 M KNO3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.04mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.90. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KNO3, using 0.04 M KNO3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.05mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.91. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KNO3, using 0.05 M KNO3.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.03 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.04 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.05 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 32: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

32

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.92. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KNO3, using 0.1 M KNO3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.2mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.93. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KNO3, using 0.2 M KNO3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.3mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.94. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KNO3, using 0.3 M KNO3.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.2 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 33: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

33

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.4mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.95. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5KNO3, using 0.4 M KNO3.

Variation of ZnSO4

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.01mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.96. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5ZnSO4, using 0.01 M ZnSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.03mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.97. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5ZnSO4, using 0.03 M ZnSO4.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + KNO3 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZNSO4 0.01 M

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.03 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 34: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

34

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.04mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.98. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5ZnSO4, using 0.04 M ZnSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.05mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.99. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5ZnSO4, using 0.05 M ZnSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.100. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5ZnSO4, using 0.1 M ZnSO4.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.04 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.05 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.1 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 35: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

35

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.101. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5ZnSO4, using 0.2 M ZnSO4.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.3mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.102. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5ZnSO4, using 0.3 M ZnSO4.

Figure S.I.103. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5ZnSO4, using 0.4 M ZnSO4.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.2 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.3 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0,1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.4mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)0.1 1 10 100

100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + ZnSO4 0.4 mL

G' i

n Pa

G''

in P

a

f in Hz

G' G''

Page 36: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

36

Variation of Ca(NO3)2

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ca(NO3)2 0.01 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.104. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ca(NO3)2, using 0.01 M Ca(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ca(NO3)2 0.03 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.105. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ca(NO3)2, using 0.03 M Ca(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ca(NO3)2 0.04 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.106. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ca(NO3)2, using 0.04 M Ca(NO3)2.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.01 M CaN2O6

G' i

n Pa

G''

in P

a

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.03 mL CaN2O6

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.04 mL CaN2O6

G' a

nd G

'' (P

a)

f in Hz

G' G''

Page 37: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

37

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ca(NO3)2 0.05 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.107. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ca(NO3)2, using 0.05 M Ca(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ca(NO3)2 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.108. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ca(NO3)2, using 0.1 M Ca(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ca(NO3)2 0.2 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.109. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ca(NO3)2, using 0.2 M Ca(NO3)2.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.05 mL CaN2O6

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.1 mL CaN2O6

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.2 mL CaN2O6

G' a

nd G

'' (P

a)

f in Hz

G' G''

Page 38: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

38

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ca(NO3)2 0.3 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.110. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ca(NO3)2, using 0.3 M Ca(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ca(NO3)2 0.4 mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.111. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ca(NO3)2, using 0.4 M Ca(NO3)2.

Variation of Ba(NO3)2

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ba(NO3)2 0.01mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.112. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ba(NO3)2, using 0.01 M Ba(NO3)2.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.3 mL CaN2O6

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.4 mL CaN2O6

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Ba(NO3)2 0.01 M

G' a

nd G

'' (P

a)

f in Hz

Page 39: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

39

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ba(NO3)2 0.03mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.113. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ba(NO3)2, using 0.03 M Ba(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ba(NO3)2 0.04mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.114. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ba(NO3)2, using 0.04 M Ba(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ba(NO3)2 0.05mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.115. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ba(NO3)2, using 0.05 M Ba(NO3)2.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.03 mL Ba(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.04 mL Ba(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.05 mL Ba(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

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40

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ba(NO3)2 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%)

Figure S.I.116. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ba(NO3)2, using 0.1 M Ba(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ba(NO3)2 0.2mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.117. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ba(NO3)2, using 0.2 M Ba(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ba(NO3)2 0.3mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.118. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ba(NO3)2, using 0.3 M Ba(NO3)2.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.1 mL Ba(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.2 mL Ba(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.3 mL Ba(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

Page 41: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

41

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Ba(NO3)2 0.4mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.119. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Ba(NO3)2, using 0.4 M Ba(NO3)2.

Variation of Sr(NO3)2

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Sr(NO3)2 0.01mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.120. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Sr(NO3)2, using 0.01 M Sr(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Sr(NO3)2 0.03mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.121. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Sr(NO3)2, using 0.03 M Sr(NO3)2.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.4 mL Ba(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

G' G''

Clay 5% + Polymer 5mg + Sr(NO3)2 0.01 M

G' a

nd G

'' (P

a)

f in Hz

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.03 mL Sr(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

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42

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Sr(NO3)2 0.04mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.122. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Sr(NO3)2, using 0.04 M Sr(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Sr(NO3)2 0.05mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.123. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Sr(NO3)2, using 0.05 M Sr(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Sr(NO3)2 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.124. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Sr(NO3)2, using 0.1 M Sr(NO3)2.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.04 mL Sr(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.05 mL Sr(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.1 mL Sr(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

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43

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Sr(NO3)2 0.2mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.125. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Sr(NO3)2, using 0.2 M Sr(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Sr(NO3)2 0.3mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.126. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Sr(NO3)2, using 0.3 M Sr(NO3)2.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Sr(NO3)2 0.4mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.127. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Sr(NO3)2, using 0.4 M Sr(NO3)2.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.2 mL Sr(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.3 mL Sr(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.4 mL Sr(NO3)2

G' a

nd G

'' (P

a)

f in Hz

G' G''

Page 44: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

44

Variation of Al2(SO4)3

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Al2(SO4)3 0.01mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.128. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Al2(SO4)3, using 0.01 M Al2(SO4)3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Al2(SO4)3 0.03mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.129. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Al2(SO4)3, using 0.03 M Al2(SO4)3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Al2(SO4)3 0.04mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.130. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Al2(SO4)3, using 0.04 M Al2(SO4)3.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.01M Al2(SO4)3

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.03 mL Al2(SO4)3

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.04 mL Al2(SO4)3

G' a

nd G

'' (P

a)

f in Hz

G' G''

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45

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Al2(SO4)3 0.05mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.131. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Al2(SO4)3, using 0.05 M Al2(SO4)3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Al2(SO4)3 0.1mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.132. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Al2(SO4)3, using 0.1 M Al2(SO4)3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Al2(SO4)3 0.2mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.133. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Al2(SO4)3, using 0.2 M Al2(SO4)3.

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.05 mL Al2(SO4)3

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.1 mL Al2(SO4)3

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.2 mL Al2(SO4)3

G' a

nd G

'' (P

a)

f in Hz

G' G''

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46

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Al2(SO4)3 0.3mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.134. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Al2(SO4)3, using 0.3 M Al2(SO4)3.

0.1 1 10 100 1000100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + Al2(SO4)3 0.4mL

G' G''

G' a

nd G

'' (P

a)

Strain (%) Figure S.I.135. Data obtained on Strain Sweep test (left) and Frequency Sweep test (right) for HN5Al2(SO4)3, using 0.4 M Al2(SO4)3.

SAXS data

Figure S.I.136. SAXS data obtained for HN5PBS (black dots), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=2.2 (blue line).

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.3 mL Al2(SO4)3

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.1 1 10 100100

101

102

103

104

105

106

Clay 5% + Polymer 5mg + 0.4 mL Al2(SO4)3

G' a

nd G

'' (P

a)

f in Hz

G' G''

0.01 0.1 1105

106

107

108

109

1010

1011

HN5PBS fit

I (a.

u.)

q (angstroms-1)

Page 47: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

47

Figure S.I.137. SAXS data obtained for HN5NaI (black dots), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=1.9 (blue line).

Figure S.I.138. SAXS data obtained for HN5Na2SO4 (black dots), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=2.0 (blue line).

Figure S.I.139. SAXS data obtained for HN5KCl (black dots), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=2.2 (blue line).

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5NaI fit

I (

a.u)

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5Na2SO4

fit

I (a.

u)

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5KCl fit

I (a.

u)

Page 48: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

48

Figure S.I.140. SAXS data obtained for HN5KNO3 (black dots), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=2.1 (blue line).

Figure S.I.141. SAXS data obtained for HN5MgSO4 (black dots), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=2.8 (blue line).

Figure S.I.142. SAXS data obtained for HN5Ba(NO3)2 (black dots), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=2.6 (blue line).

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5KNO3

fit

I (

a.u)

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5MgSO4

fit

I (a.

u)

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5Ba(NO3)2

fit

I (a.

u)

Page 49: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

49

Figure S.I.143. SAXS data obtained for HN5Sr(NO3)2 (black dots), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=2.7 (blue line).

Figure S.I.144. SAXS data obtained for HN5CuSO4 (black dots), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=3.2 (blue line).

Figure S.I.145. SAXS data obtained for HN5ZnSO4 (black dots), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=3.1 (blue line).

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5Sr(NO3)2

fit

I (

a.u)

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5CuSO4

fit

I (a.

u)

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5ZnSO4

fit

I (a.

u)

Page 50: SI - Hydrogels1 Supporting Information Structure-Property Relationship in Laponite Materials: From Wigner Glasses to Strong Self-Healing Hydrogels Formed by Non-Covalent Interactions

50

Figure S.I.146. SAXS data obtained for HN5Ca(NO3)4 (in blue), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=3.31.

Figure S.I.147. SAXS data obtained for HN5Al2(SO4)3 (in blue), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=3.0.

Figure S.I.148. SAXS data obtained for HN5CeCl3 (in blue), and fit curve obtained on SASFit for a model of a monodisperse flat cylinder with 9.5 nm radius, 0.9 nm width and a mass fractal structure with D=2.8.

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5Ca(NO3)2

fit

I (

a.u)

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5Al2(SO4)3

fit

I (a.

u)

0.01 0.1 1105

106

107

108

109

1010

1011

q (angstroms-1)

HN5CeCl3 fit

I (a.

u)