Slide-ring materials are polymer networks with mobile
cross-links
that exhibit impressive stress dissipation and fracture resistance
owing to the pulley effect. On account of their remarkable ability
to dissipate the energy of deformation, these materials have found
their way into advanced materials such as abrasion-resistant coatings
and elastic battery electrode binders. In this work, we explore the
role of mobile cross-links on the properties of a biofriendly pressure-sensitive
adhesive made using composites of cyclodextrin-based macromolecules
and poly(lipoic acid). We modify cyclodextrin-based hosts and polyrotaxanes
with pendant groups of lipoic acid (a commonly ingested antioxidant)
to incorporate them as cross-links in poly(lipoic acid) networks obtained
by simple heating in open air. By systematically varying the adhesive
formulations while probing their mechanical and adhesive properties,
we uncover trends in structure–property relationships that
enable one to tune network properties and access biofriendly, high-tack
adhesives.