| Title | Esterase Cleavable 2D Assemblies of Magnetic Iron Oxide Nanocubes: Exploiting Enzymatic Polymer Disassembling to Improve Magnetic Hyperthermia Heat Losses |
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| Type | Journal article |
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| Authors | Avugadda, S.K., Materia, M.E., Nigmatullin, R., Cabrera, D., Marotta, R., Cabada, T.F., Marcello, E., Nitti, S., Artés-Ibañez, E.J., Basnett, P., Wilhelm, C., Teran, F.J., Roy, I. and Pellegrino, T. |
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| Abstract | Here, we report a nanoplatform based on iron oxide nanocubes (IONCs) coated with a bioresorbable polymer that, upon exposure to lytic enzymes can be disassembled increasing the heat performances in comparison with the initial clusters. We have developed bi-dimensional (2D) clusters by exploiting benchmark iron oxide nanocubes as heat mediators for magnetic hyperthermia and a polyhydroxyalkanoate (PHA) copolymer, a biodegradable polymer produced by bacteria that can be digested by intracellular esterase enzymes. The comparison of magnetic heat performance of the 2D assemblies with 3D centro-symmetrical assemblies or single iron oxide nanocubes emphasize the benefit of the 2D assembly. On one hand, the heat losses of 2D assemblies dispersed in water are better than the 3D assemblies, but worse than for single nanocubes. On the other hand, when the bi-dimensional magnetic beads (2D-MNBs) are incubated with the esterase enzyme at a physiological temperature, their magnetic heat performances began to progressively increase. After 2 hours of incubation, specific absorption rate values of the 2D assembly double the ones of individually coated nanocubes. Such an increase can be mainly correlated to the splitting of the 2D-MNBs into smaller size clusters with a chain- like configuration containing few nanocubes. Moreover, 2D-MNBs exhibited non-variable-heat performances even after intentionally inducing their aggregation. Magnetophoresis measurements indicate a comparable response of 3D and 2D clusters to external magnets (0.3T) that is by far faster than that of single nanocubes. This feature is crucial for a physical accumulation of magnetic materials in the presence of magnetic field gradients. This system is the first example of a nanoplatform that, upon exposure to lytic enzymes, such as those present in a tumor environment, can be disassembled from the initial 2D-MNB organization to chain-like assemblies with clear improvement of the heat magnetic losses resulting in better heat dissipation performances. The potential application of 2D nano-assemblies based on the cleavable PHAs for preserving their magnetic losses inside cells will benefit hyperthermia therapies mediated by magnetic nanoparticles under alternating magnetic fields. |
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| Keywords | Polyhydroxyalkanoates |
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| Journal | Chemistry of Materials |
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| Journal citation | 31 (15), pp. 5450-5463 |
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| ISSN | 0897-4756 |
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| Year | 2019 |
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| Publisher | American Chemical Society |
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| Accepted author manuscript | |
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| Digital Object Identifier (DOI) | https://doi.org/10.1021/acs.chemmater.9b00728 |
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| Publication dates |
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| Published online | 26 Jun 2019 |
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