Peptide-mediated Al(III) (oxy)(hydr)oxide formation

the specific stages of phase separation for additive interactions matter

verfasst von

Miodrag J. Lukić, Nele Marquardt, Tim Schmalz, Denis Gebauer

Abstract

We demonstrate how Al(III) interactions with a ‘biomimetic’ model homo-peptide, polyaspartic (pAsp), with a narrow size distribution (around 20 amino acid monomer units), can lead to substantially different outcomes by governing Al(III) hydrolysis/phase separation. The addition of unhydrolysed Al(III) in aqueous peptide solutions results in dominant pAsp20 destabilisation and precipitation from the solution, failing to induce effective Al(III)(oxy)(hydr)oxide formation. Allowing the peptide-free Al(III) system to reach specific hydrolysis/phase separation stages, i.e., just before and slightly after liquid-liquid phase separation, partly dissipating its chemical energy, followed by controlled peptide addition, leads to the formation of respective Al(III)(oxy)(hydr)oxide-peptide hybrids with smaller particles, higher Al(III) content, and well-preserved chemical properties of the peptide. This constitutes a hydrolysis “spin-off” strategy that exploits Al(III)-peptide interactions in distinct hydrolytic precursors, an approach transferable to multiple metals and polymeric systems. The reaction energetics determined by revisited isothermal titration calorimetry assays reflect an Al(III) hydrolysis “footprint” and its role in metal-peptide interactions. These insights are important for various applications of aluminium species, from vaccine adjuvants and related toxicity to enhancements of corrosion resistance.

Organisationseinheit(en)

Institut für Anorganische Chemie
Institut für Radioökologie und Strahlenschutz

Externe Organisation(en)

University of Belgrade

Typ

Artikel

Journal

Inorganic chemistry frontiers

Band

12

Seiten

6235-6245

Anzahl der Seiten

11

ISSN

2052-1545

Publikationsdatum

07.10.2025

Publikationsstatus

Veröffentlicht

Peer-reviewed

Ja

ASJC Scopus Sachgebiete

Anorganische Chemie

Ziele für nachhaltige Entwicklung

SDG 3 – Gute Gesundheit und Wohlergehen

Elektronische Version(en)

https://doi.org/10.1039/d5qi00870k (Zugang: Offen)