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Layer-by-Layer Coatings of Collagen-Hyaluronic acid Loaded with an Antibacterial Manuka Honey Bioactive Compound to Fight Metallic Implant Infections

Lookup NU author(s): Dr Anjaneyulu Udduttulla, Professor Nicholas JakubovicsORCiD, Dr Kenneth RankinORCiD, Dr Piergiorgio GentileORCiD, Dr Ana Ferreira-DuarteORCiD



This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).


© 2023 The Authors. Published by American Chemical Society. Implant-associated severe infections can result in catastrophic implant failures; thus, advanced antibacterial coatings are needed to combat infections. This study focuses on harnessing nature-inspired self-assembly of extracellular matrix (ECM)-like coatings on Ti alloy with a combination of jellyfish-derived collagen (J-COLL) and hyaluronic acid (HA) using our customized automated hybrid layer-by-layer apparatus. To improve the anti-infection efficacy of coatings, we have incorporated a natural antibacterial agent methylglyoxal (MGO, a Manuka honey compound) in optimized multilayer coatings. The obtainment of MGO-loaded multilayer coatings was successfully assessed by profilometry, contact angle, attenuated total reflectance (ATR)-Fourier transform infrared spectroscopy, scanning electron microscopy, and X-ray photoelectron spectroscopy. In vitro degradation confirmed the controlled release activity of MGO with a range of concentrations from 0.90 to 2.38 mM up to 21 days. A bacterial cell culture study using Escherichia coli (E. coli) and Staphylococcus epidermidis (S. epidermidis) confirmed that the MGO incorporated within layers 7 and 9 had a favorable effect on preventing bacterial growth and colonization on their surfaces. An in vitro cytocompatibility study confirmed that MGO agents included in the layers did not affect or reduce the cellular functionalities of L929 fibroblasts. In addition, MGO-loaded layers with Immortalized Mesenchymal Stem Cells (Y201 TERT-hMSCs) were found to favor the growth and differentiation of Y201 cells and promote calcium nodule formation. Overall, these surface coatings are promising candidates for delivering antimicrobial activity with bone-inducing functions for future bone tissue engineering applications.

Publication metadata

Author(s): Udduttula A, Jakubovics N, Khan I, Pontiroli L, Rankin KS, Gentile P, Ferreira AM

Publication type: Article

Publication status: Published

Journal: ACS Applied Materials and Interfaces

Year: 2023

Volume: 15

Issue: 50

Pages: 58119-58135

Print publication date: 20/12/2023

Online publication date: 06/12/2023

Acceptance date: 16/11/2023

Date deposited: 05/02/2024

ISSN (print): 1944-8244

ISSN (electronic): 1944-8252

Publisher: American Chemical Society


DOI: 10.1021/acsami.3c11910


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Funder referenceFunder name
the National Institute for Health and Care Research (NIHR)
the Orthopaedic Research United Kingdom (ORUK #536)