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Abstract
Metal oxide nanoparticles have emerged as exceptionally potent biomedical sensors and actuators due to their unique physicochemical features. Despite fascinating achievements, the current limited understanding of the molecular interplay between nanoparticles and the surrounding tissue remains a major obstacle in the rationalized development of nanomedicines, which is reflected in their poor clinical approval rate. This work reports on the nanoscopic characterization of inorganic nanoparticles in tissue by the example of complex metal oxide nanoparticle hybrids consisting of crystalline cerium oxide and the biodegradable ceramic bioglass. A validated analytical method based on semiquantitative X‐ray fluorescence and inductively coupled plasma spectrometry is used to assess nanoparticle biodistribution following intravenous and topical application. Then, a correlative multiscale analytical cascade based on a combination of microscopy and spectroscopy techniques shows that the topically applied hybrid nanoparticles remain at the initial site and are preferentially taken up into macrophages, form apatite on their surface, and lead to increased accumulation of lipids in their surroundings. Taken together, this work displays how modern analytical techniques can be harnessed to gain unprecedented insights into the biodistribution and biotransformation of complex inorganic nanoparticles. Such nanoscopic characterization is imperative for the rationalized engineering of safe and efficacious nanoparticle‐based systems.
Highlights
Metal oxide nanoparticles have emerged as exceptionally potent biomedical sensors and actuators due to their unique physicochemical features
We demonstrate how information on the fate of nanoparticles can be obtained by retrieving molecular fingerprint information using a combination of hyperspectral Raman spectroscopy mapping, time-of-flight secondary ion mass spectrometry (TOFSIMS) imaging and density-dependent color scanning electron microscopy (DDC-SEM), bridging the aforementioned localization gap
The techniques utilized for the as-prepared characterization of this complex system are applicable to a wide range of inorganic nanoparticles
Summary
Metal oxide nanoparticles have emerged as exceptionally potent biomedical sensors and actuators due to their unique physicochemical features. While some metal oxide nanoparticles have received market approval,[17] especially as imaging agents,[18] their translation has been slow in recent years.[19,20] For many metal oxide nanosystems there are safety concerns regarding their poor degradability and the limited understanding of their in vivo fate.[21,22] The detailed understanding of the interactions of nanoparticles with biological entities, especially their redistribution and degradation, remains pivotal for the safe and efficacious development of nanoparticlebased products in general.[23] The inability to measure and assess this interplay renders both improvement and regulation of nanomedicine extremely challenging. We selected complex nanoparticles used as tissue adhesives as an analytically very challenging but medically relevant material to showcase the opportunities and limitations of the proposed analytical imaging cascade These metal oxide nanoparticle hybrids consisting of bioglass and ceria (BG/ceria) were applied either topically as tissue glues to the subcutis in a rat skin flap model or systemically. Such in-depth characterization and analysis provide additional insights into the material-biology interplay, which are inaccessible by conventional methods (histological and immunological assays and elemental analysis) and will support the rational development and regulation of a wide range of nanomaterials for biomedical applications
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