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Elastic-Modulus-Dependent Macroscopic Supramolecular Assembly of Poly(dimethylsiloxane) for Understanding Fast

Yingzhi Sun¹, Xinghuan Wang¹, Menglin Xiao¹

¹State Key Laboratory of Chemical Resource Engineering & Beijing Laboratory of Biomedical Materials & Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China.

Langmuir : the ACS Journal of Surfaces and Colloids

|April 1, 2021

Summary

Macroscopic supramolecular assembly (MSA) is now possible in non-hydrogel elastomers by tuning their elastic modulus. Lower modulus materials show higher assembly probability, enabling new applications in adhesion and additive manufacturing.

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Area of Science:

Supramolecular Chemistry
Materials Science

Background:

Macroscopic supramolecular assembly (MSA) utilizes noncovalent interactions for building macroscopic materials.
Current MSA is primarily limited to hydrogels due to requirements for molecular mobility.
Extending MSA to diverse materials like elastomers is crucial for broader applications.

Purpose of the Study:

To develop a strategy for realizing MSA in nonhydrogel materials by adjusting intrinsic properties.
To investigate the relationship between elastic modulus and MSA probability in elastomers.
To broaden the scope of materials amenable to macroscopic supramolecular assembly.

Main Methods:

Adjusting the elastic modulus of poly(dimethylsiloxane) (PDMS) elastomers.
Utilizing host/guest molecular recognition (β-cyclodextrin and adamantane) for noncovalent interactions.
Quantifying MSA probability across a range of elastic moduli (0.38–3.84 MPa).
Performing in situ measurements of interactive forces between building blocks.

Main Results:

Demonstrated elastic-modulus-dependent MSA in PDMS elastomers.
MSA probability decreased from 100% at 0.38 MPa to 0% at 3.84 MPa.
In situ force measurements confirmed assembly phenomena and supported the multivalency theory.
Low-modulus flexible surfaces enhance molecular mobility for interfacial interactions.

Conclusions:

Achieved MSA in nonhydrogel elastomers by directly adjusting the elastic modulus.
This approach broadens material choices for MSA.
Findings offer insights into fast wet adhesion and additive manufacturing of elastomers.