Polyoxometalate-polypeptide nanoassemblies as peroxidase surrogates with antibiofilm properties

Soria-Carrera, H. ; Atrián-Blasco, E. ; de la Fuente, J. M. ; Mitchell, S. G. ; Martín-Rapún, R. (Universidad de Zaragoza)

Resumen: Developing artificial metalloenzymes that possess a superior performance to their natural counterparts is an attractive concept. Polyoxometalates (POMs) are a class of anionic molecular metal-oxides with excellent redox properties and bioactivity. We have recently introduced “POMlymers” - covalently conjugated POM-peptide hybrid materials - where the polypeptide chain is obtained through a ring-opening polymerisation (ROP) of a-amino acid N-carboxyanhydrides (NCA) on an inorganic POM scaffold. Attracted by the idea of preparing artificial metalloenzymes, here we report the supramolecular self-assembly of POMlymer hybrids into nanoparticles where an optimal environment for catalysis is created. Our results demonstrate that the self-assembly of covalent POMlymers, enhances the peroxidase-like activity of the parent POM anion whereas, in contrast, the catalytic activity for nanoparticles obtained by ionic self-assembly of the same peptide and POM components practically disappears. Furthermore, POMlymer nanoparticles also present antimicrobial and antibiofilm activity against the skin bacterium Staphylococcus epidermidis; whereas, ionic POM-peptide hybrids significantly increase biofilm production and endogenous production of reactive oxygen species. In summary, we present the self-assembly of POMlymer hybrids into nanoparticles and a combination of peroxidase activity and microbiology assays that show that the POM-peptide covalent bond is essential for the stability of the self-assembled nanoparticles and therefore for their catalytic and biological activity. © 2022 The Royal Society of Chemistry.

Idioma: Inglés

DOI: 10.1039/d1nr08223j

Año: 2022

Publicado en: Nanoscale 14, 16 (2022), 5999-6006
ISSN: 2040-3364

Factor impacto JCR: 6.7 (2022)

Categ. JCR: MATERIALS SCIENCE, MULTIDISCIPLINARY rank: 83 / 343 = 0.242 (2022) - Q1 - T1
Categ. JCR: PHYSICS, APPLIED rank: 27 / 160 = 0.169 (2022) - Q1 - T1
Categ. JCR: CHEMISTRY, MULTIDISCIPLINARY rank: 43 / 178 = 0.242 (2022) - Q1 - T1
Categ. JCR: NANOSCIENCE & NANOTECHNOLOGY rank: 37 / 107 = 0.346 (2022) - Q2 - T2

Factor impacto CITESCORE: 13.6 - Materials Science (Q1)

Factor impacto SCIMAGO: 1.62 - Nanoscience and Nanotechnology (Q1) - Materials Science (miscellaneous) (Q1)

Financiación: info:eu-repo/grantAgreement/ES/CSIC/i-Link+2019-LINK20270
Financiación: info:eu-repo/grantAgreement/ES/DGA/E15-20R
Financiación: info:eu-repo/grantAgreement/EC/H2020/845427/EU/Peptide-functionalized POMs as biofilm disruption agents: searching for synergy in bactericidal materials/PePiPOM
Financiación: info:eu-repo/grantAgreement/ES/MEC/FPU2016-02456
Financiación: info:eu-repo/grantAgreement/ES/MICINN/PID2019-109333RB-I00

Tipo y forma: Article (Published version)

Área (Departamento): Área Química Orgánica (Dpto. Química Orgánica)