TY - JOUR
T1 - 4d multimodal nanomedicines made of nonequilibrium au-fe alloy nanoparticles
AU - Amendola, Vincenzo
AU - Torresan, Veronica
AU - Forrer, Daniel
AU - Guadagnini, Andrea
AU - Badocco, Denis
AU - Pastore, Paolo
AU - Casarin, Maurizio
AU - Selloni, Annabella
AU - Coral, Diego
AU - Ceolin, Marcelo
AU - Fernandez Van Raap, Marcela B.
AU - Busato, Alice
AU - Marzola, Pasquina
AU - Spinelli, Antonello E.
N1 - Funding Information:
We would like to acknowledge M. Gerosa of Verona University for help with MRI measurements in phantoms, L. Perani (San Raffaele Preclinical Imaging Facility) for the support with the animal handling, and F. Amleto (San Raffaele Mouse Histopathology Unit) for the support with the histological analysis. This research was funded by the University of Padova STARS grant “4NANOMED” and the Italian Ministry of Foreign Affairs and International Cooperation “Great relevance project” with protocol number 0191594. D.F. acknowledges the support by the CNR Short-Term mobility program 2018. We acknowledge the CINECA award under the ISCRA initiative, the TIGRESS high performance computer center at Princeton University, and the C3P computer facility at the University of Padova.
Publisher Copyright:
© 2020 American Chemical Society.
PY - 2020/10/27
Y1 - 2020/10/27
N2 - Several examples of nanosized therapeutic and imaging agents have been proposed to date, yet for most of them there is a low chance of clinical translation due to longterm in vivo retention and toxicity risks. The realization of nanoagents that can be removed from the body after use remains thus a great challenge. Here, we demonstrate that nonequilibrium gold-iron alloys behave as shape-morphing nanocrystals with the properties of self-degradable multifunctional nanomedicines. DFT calculations combined with mixing enthalpy-weighted alloying simulations predict that Au-Fe solid solutions can exhibit self-degradation in an aqueous environment if the Fe content exceeds a threshold that depends upon element topology in the nanocrystals. Exploiting a laserassisted synthesis route, we experimentally confirm that nonequilibrium Au-Fe nanoalloys have a 4D behavior, that is, the ability to change shape, size, and structure over time, becoming ultrasmall Au-rich nanocrystals. In vivo tests show the potential of these transformable Au-Fe nanoalloys as efficient multimodal contrast agents for magnetic resonance imaging and computed X-ray absorption tomography and further demonstrate their self-degradation over time, with a significant reduction of long-term accumulation in the body, when compared to benchmark gold or iron oxide contrast agents. Hence, Au-Fe alloy nanoparticles exhibiting 4D behavior can respond to the need for safe and degradable inorganic multifunctional nanomedicines required in clinical translation.
AB - Several examples of nanosized therapeutic and imaging agents have been proposed to date, yet for most of them there is a low chance of clinical translation due to longterm in vivo retention and toxicity risks. The realization of nanoagents that can be removed from the body after use remains thus a great challenge. Here, we demonstrate that nonequilibrium gold-iron alloys behave as shape-morphing nanocrystals with the properties of self-degradable multifunctional nanomedicines. DFT calculations combined with mixing enthalpy-weighted alloying simulations predict that Au-Fe solid solutions can exhibit self-degradation in an aqueous environment if the Fe content exceeds a threshold that depends upon element topology in the nanocrystals. Exploiting a laserassisted synthesis route, we experimentally confirm that nonequilibrium Au-Fe nanoalloys have a 4D behavior, that is, the ability to change shape, size, and structure over time, becoming ultrasmall Au-rich nanocrystals. In vivo tests show the potential of these transformable Au-Fe nanoalloys as efficient multimodal contrast agents for magnetic resonance imaging and computed X-ray absorption tomography and further demonstrate their self-degradation over time, with a significant reduction of long-term accumulation in the body, when compared to benchmark gold or iron oxide contrast agents. Hence, Au-Fe alloy nanoparticles exhibiting 4D behavior can respond to the need for safe and degradable inorganic multifunctional nanomedicines required in clinical translation.
KW - Alloys
KW - Au nanoparticles
KW - CT
KW - Degradable materials
KW - Fe nanoparticles
KW - MRI
KW - Nanomedicine
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U2 - 10.1021/acsnano.0c03614
DO - 10.1021/acsnano.0c03614
M3 - Article
C2 - 32877170
AN - SCOPUS:85094983931
SN - 1936-0851
VL - 14
SP - 12840
EP - 12853
JO - ACS Nano
JF - ACS Nano
IS - 10
ER -