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Iron-based trinuclear metal-organic nanostructures on a surface with local charge accumulation.

ABSTRACT: Coordination chemistry relies on harnessing active metal sites within organic matrices. Polynuclear complexes-where organic ligands bind to several metal atoms-are relevant due to their electronic/magnetic properties and potential for functional reactivity pathways. However, their synthesis remains challenging; few geometries and configurations have been achieved. Here, we synthesise-via supramolecular chemistry on a noble metal surface-one-dimensional metal-organic nanostructures composed of terpyridine (tpy)-based molecules coordinated with well-defined polynuclear iron clusters. Combining low-temperature scanning probe microscopy and density functional theory, we demonstrate that the coordination motif consists of coplanar tpy's linked via a quasi-linear tri-iron node in a mixed (positive-)valence metal-metal bond configuration. This unusual linkage is stabilised by local accumulation of electrons between cations, ligand and surface. The latter, enabled by bottom-up on-surface synthesis, yields an electronic structure that hints at a chemically active polynuclear metal centre, paving the way for nanomaterials with novel catalytic/magnetic functionalities.

SUBMITTER: Krull C

PROVIDER: S-EPMC6086834 | biostudies-literature | 2018 Aug

REPOSITORIES: biostudies-literature

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Iron-based trinuclear metal-organic nanostructures on a surface with local charge accumulation.

Krull Cornelius C Castelli Marina M Hapala Prokop P Kumar Dhaneesh D Tadich Anton A Capsoni Martina M Edmonds Mark T MT Hellerstedt Jack J Burke Sarah A SA Jelinek Pavel P Schiffrin Agustin A

Nature communications 20180810 1

Coordination chemistry relies on harnessing active metal sites within organic matrices. Polynuclear complexes-where organic ligands bind to several metal atoms-are relevant due to their electronic/magnetic properties and potential for functional reactivity pathways. However, their synthesis remains challenging; few geometries and configurations have been achieved. Here, we synthesise-via supramolecular chemistry on a noble metal surface-one-dimensional metal-organic nanostructures composed of te ...[more]

PMID: 30097562

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Project description:In recent years, pure iron (Fe) has attracted significant attention as a promising biodegradable orthopedic implant material due to its excellent mechanical and biological properties. However, in physiological conditions, Fe has an extremely slow degradation rate with localized and irregular degradation, which is problematic for practical applications. In this study, we developed a novel combination of a nanostructured surface topography and galvanic reaction to achieve uniform and accelerated degradation of an Fe implant. The target-ion induced plasma sputtering (TIPS) technique was applied on the Fe implant to introduce biologically compatible and electrochemically noble tantalum (Ta) onto its surface and develop surface nano-galvanic couples. Electrochemical tests revealed that the uniformly distributed nano-galvanic corrosion cells of the TIPS-treated sample (nano Ta–Fe) led to relatively uniform and accelerated surface degradation compared to that of bare Fe. Furthermore, the mechanical properties of nano Ta–Fe remained almost constant during a long-term in vitro immersion test (~40 weeks). Biocompatibility was also assessed on surfaces of bare Fe and nano Ta–Fe using in vitro osteoblast responses through direct and indirect contact assays and an in vivo rabbit femur medullary cavity implantation model. The results revealed that nano Ta–Fe not only enhanced cell adhesion and spreading on its surface, but also exhibited no signs of cellular or tissue toxicity. These results demonstrate the immense potential of Ta-implanted surface nanostructures as an effective solution for the practical application of Fe-based orthopedic implants, ensuring long-term biosafety and clinical efficacy. Graphical abstract Image 1 Highlights • The degradation rate of nanostructured Fe implants was accelerated by TIPS technique.• Ta ions were accelerated strongly toward the Fe surface by TIPS process.• Nano Ta–Fe showed long-term mechanical stability and accelerated degradation rate.• Nanostructured Ta–Fe surface showed enhanced in vitro and in vivo cellular responses.• Ta-implanted Fe is a promising material for biodegradable orthopedic implants.

Dataset Information

Iron-based trinuclear metal-organic nanostructures on a surface with local charge accumulation.

Publications

Iron-based trinuclear metal-organic nanostructures on a surface with local charge accumulation.

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