Harnessing entropy to direct the bonding/debonding of polymer systems based on reversible chemistry

Nathalie K. Guimard, Junming Ho, Josef Brandt, Ching Yeh Lin, Mansoor Namazian, Jan O. Mueller, Kim K. Oehlenschlaeger, Stefan Hilf, Albena Lederer, Friedrich G. Schmidt, Michelle L. Coote, Christopher Barner-Kowollik*

*Corresponding author for this work

    Research output: Contribution to journalArticlepeer-review

    47 Citations (Scopus)


    The widely accepted approach for controlling polymer debonding/rebonding properties in responsive materials has been to purposefully engineer the functional end-groups responsible for monomer dynamic bonding. Here, however, we evidence that the debonding temperature of a polymer can also be tuned by changing the chain length of the polymer building blocks, thus altering the entropy released on debonding. Entropy driven debonding, as governed by building block chain length, is suggested theoretically and realized experimentally for two Diels-Alder polymer systems, each based on a different difunctional diene and a common difunctional dienophile. In each case a significant decrease (as much as 60 °C) in the retro Diels-Alder temperature was observed when the chain length of the difunctional dienophile building block was increased. These results have the potential to fundamentally change the approach utilized to design materials capable of bonding reversibly on demand.

    Original languageEnglish
    Pages (from-to)2752-2759
    Number of pages8
    JournalChemical Science
    Issue number7
    Publication statusPublished - 4 Jun 2013


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