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Phosphonic acid derivatives are suitable compounds for controlling the surface properties of materials and nanomaterials. Here, we present for the first time the use of alkyl phosphonic acid ligands to transfer into water zero-valent iron nanoparticles (FeNP) synthesized by an organometallic approach. The transfer takes place with the formation of an oxide layer at the surface of the iron nanoparticles, beneficial for the coordination of the alkyl phosphonic acid ligands. The nanoparticles are highly soluble in water and present a core–shell structure, with a monocrystalline body-centered cubic iron core of ca. 10 nm in size surrounded by a spinel oxide shell of ca. 2 nm thickness. These hydrophilic nanoparticles display excellent structural stability, magnetization still reaching 70% of that of bulk iron, and a transversal relaxivity r2 of 335 mM−1 s−1 which give them high potential for biomedical applications. [ABSTRACT FROM AUTHOR]

The growing concern over the toxicity of Gd-based contrast agents used in magnetic resonance imaging (MRI) motivates the search for less toxic and more effective alternatives. Among these alternatives, iron–iron oxide (Fe@FeOx) core-shell architectures have been long recognized as promising MRI contrast agents while limited information on their engineering is available. Here we report the synthesis of 10 nm large Fe@FeOx nanoparticles, their coating with a 11 nm thick layer of dense silica and functionalization by 5 kDa PEG chains to improve their biocompatibility. The nanomaterials obtained have been characterized by a set of complementary techniques such as infra-red and nuclear magnetic resonance spectroscopies, transmission electron microscopy, dynamic light scattering and zetametry, and magnetometry. They display hydrodynamic diameters in the 100 nm range, zetapotential values around −30 mV, and magnetization values higher than the reference contrast agent RESOVIST®. They display no cytotoxicity against 1BR3G and HCT116 cell lines and no hemolytic activity against human red blood cells. Their nuclear magnetic relaxation dispersion (NMRD) profiles are typical for nanomaterials of this size and magnetization. They display high r2 relaxivity values and low r1 leading to enhanced r2/r1 ratios in comparison with RESOVIST®. All these data make them promising contrast agents to detect early stage tumors. [ABSTRACT FROM AUTHOR]