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<p>Designing sustainable polymers that self-assemble in water remains a major challenge for advanced functional materials. Here, three partially bio-based poly(amic acid) (PAA) derived from difurfurylamine-based diamines were synthezised and converted into their triethylammonium salts (PAAS) to enable aqueous processing and electrostatic assembly with a branched poly(ethyleneimine) (PEI). Structural and thermal analyses established the key physicochemical properties of the polymers. Systematic mapping of PAAS/PEI mixtures revealed three distinct regimes. Under PAAS rich conditions, only the difurfuryl di-methyl based PAAS (PAAS/DFDA-<i>DM</i>) formed stable anionic nanoparticles (NPs) (≈ 15&#xa0;nm), whereas phenyl and cyclohexane derived analogues precipitated. Near charge-stoichiometry, all systems produced dense polyelectrolyte complex (PEC) aggregates. In PEI excess compositions, all PAAS yielded well dispersed, positively charged nanoparticles (10–20&#xa0;nm), indicating that PEI overcharging governs colloidal stabilization. These findings show that backbone structure and charge accessibility critically determine PEC formation and highlight PAAS/DFDA-<i>DM</i> as the most versatile candidate for sustainable nanoparticle design.</p> Graphical abstract <p></p>

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Toward sustainable polyelectrolyte nanoparticles: aqueous self-assembly of partially bio-based poly(amic acids) with poly(ethyleneimine)

  • 期刊论文

  • 发表日期：

    2026年7月28日

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  • Lauran Mama,
  • Claudio Mortier,
  • Pierre Delliere,
  • Vincent Lapinte,
  • Sylvain Caillol,
  • Camille Bakkali-Hassani,
  • Nathalie Masquelez,
  • Damien Quemener

摘要

Designing sustainable polymers that self-assemble in water remains a major challenge for advanced functional materials. Here, three partially bio-based poly(amic acid) (PAA) derived from difurfurylamine-based diamines were synthezised and converted into their triethylammonium salts (PAAS) to enable aqueous processing and electrostatic assembly with a branched poly(ethyleneimine) (PEI). Structural and thermal analyses established the key physicochemical properties of the polymers. Systematic mapping of PAAS/PEI mixtures revealed three distinct regimes. Under PAAS rich conditions, only the difurfuryl di-methyl based PAAS (PAAS/DFDA-DM) formed stable anionic nanoparticles (NPs) (≈ 15 nm), whereas phenyl and cyclohexane derived analogues precipitated. Near charge-stoichiometry, all systems produced dense polyelectrolyte complex (PEC) aggregates. In PEI excess compositions, all PAAS yielded well dispersed, positively charged nanoparticles (10–20 nm), indicating that PEI overcharging governs colloidal stabilization. These findings show that backbone structure and charge accessibility critically determine PEC formation and highlight PAAS/DFDA-DM as the most versatile candidate for sustainable nanoparticle design.

Graphical abstract