Ligand biodegradation-induced surface reconstruction of magnetite nanoparticles: potentially overlooked toxicity. Issue 1 (10th December 2021)

• Record Type: Journal Article
• Authors: Zhao, Huiru; Meng, Hongyan; Zhang, Qiurong; Wu, Yining; Chen, Haotian; Jiang, Xiaoman; Zhang, Chengdong
• Is Part Of: Environmental science. Volume 9:Issue 1(2022)
• Page Start: 313
• Page End: 323
• Publication Date: 2021-12-10
• Subjects: Environmental sciences -- Periodicals; Nanotechnology -- Periodicals; 620.505
• DOI: 10.1039/d1en00724f
• Languages: English
• ISSNs: 2051-8153

Abstract

Abstract : The coating of nanoparticles (NPs) with biodegradable ligands has been considered an efficient way to improve the biocompatibility of NPs and to decrease their biopersistence. Abstract : The coating of nanoparticles (NPs) with biodegradable ligands has been considered an efficient way to improve the biocompatibility of NPs and to decrease their biopersistence. However, the role of ligand biodegradation in reshaping the core material and the resulting change in toxicity have not been fully explored. In this study, magnetite (Fe3 O4 ) NPs coated with a high or low loading of hyaluronic acid (termed Fe3 O4 –HAH and Fe3 O4 –HAL ) were synthesized. Fe3 O4 –HAR was obtained after the enzymatic degradation of Fe3 O4 –HAH by a hyaluronidase, which had a coating weight similar to that of Fe3 O4 –HAL, as verified by thermogravimetric analysis. Interestingly, among the three NPs, Fe3 O4 –HAR induced the highest rate of cellular damage. In particular, 2 times more hydroxyl radicals were detected in cells stressed by Fe3 O4 –HAR than in cells stressed by Fe3 O4 –HAH, despite the highest cellular uptake being observed for Fe3 O4 –HAH because of the ligand–receptor interactions between hyaluronic acid and membrane receptors. The structural characterization results revealed that ligand degradation induced notable surface reconstruction of the Fe3 O4 core, showing a characteristic Fe3 O4 @Fe2 O3 structure with surface-bound ferrous ions. This unique structure endowed Fe3 O4 –HAR with superior competency in initiating the Fenton reaction and accelerating the Fe(iii )/Fe(ii ) cycle. Our results emphasize the importance of tracing the in vivo biotransformation of NPs from all of the different architectural parts, particularly deciphering the interplay among the core, shell, surface ligands, and surrounding ions.