van Lange Sophie G M, Te Brake Diane W, Portale Giuseppe, Palanisamy Anbazhagan, Sprakel Joris, van der Gucht Jasper
Physical Chemistry and Soft Matter, Wageningen University and Research, 6708 WE Wageningen, Netherlands.
Macromolecular Chemistry and New Polymeric Materials, Zernike Institute for Advanced Materials, University of Groningen, 9747 AG Groningen, Netherlands.
Sci Adv. 2024 Jan 12;10(2):eadi3606. doi: 10.1126/sciadv.adi3606. Epub 2024 Jan 10.
While nature extensively uses electrostatic bonding between oppositely charged polymers to assemble and stabilize materials, harnessing these interactions in synthetic systems has been challenging. Synthetic materials cross-linked with a high density of ionic bonds, such as polyelectrolyte complexes, only function properly when their charge interactions are attenuated in the presence of ample amounts of water; dehydrating these materials creates such strong Coulombic bonding that they become brittle, non-thermoplastic, and virtually impossible to process. We present a strategy to intrinsically moderate the electrostatic bond strengths in apolar polymeric solids by the covalent grafting of attenuator spacers to the charge carrying moieties. This produces a class of polyelectrolyte materials that have a charge density of 100%, are processable and malleable without requiring water, are highly solvent- and water-resistant, and are fully recyclable. These materials, which we coin "compleximers," marry the properties of thermoplastics and thermosets using tailored ionic bonding alone.
虽然自然界广泛利用带相反电荷的聚合物之间的静电键合来组装和稳定材料，但在合成体系中利用这些相互作用一直具有挑战性。与高密度离子键交联的合成材料，如聚电解质复合物，只有在大量水存在下其电荷相互作用减弱时才能正常发挥作用；使这些材料脱水会产生如此强的库仑键，以至于它们变得易碎、非热塑性且几乎无法加工。我们提出了一种策略，通过将衰减剂间隔基共价接枝到带电部分，在非极性聚合物固体中内在地调节静电键强度。这产生了一类聚电解质材料，其电荷密度为100%，无需水即可加工和延展，具有高度的耐溶剂性和耐水性，并且完全可回收。我们将这些材料称为“复合聚合物”，仅通过定制的离子键合就兼具了热塑性塑料和热固性塑料的特性。
