We report the design of a unique bioinspired ligand merging redox-active catechol and flavin-related alloxazine substructures.Upon coordination with a Ni_((II))salt,this hybrid ligand forms a trinuclear complex contai...We report the design of a unique bioinspired ligand merging redox-active catechol and flavin-related alloxazine substructures.Upon coordination with a Ni_((II))salt,this hybrid ligand forms a trinuclear complex containing three NiII centers and three redox-active ligands.This air-stable metallic triangle stabilizing protons and electrons was studied by X-ray crystallography,infra-red(IR)and UV-vis spectroscopy,SQUID magnetometry(Superconducting QUantum Interference Device),MAS-NMR(Magic Angle Spinning-Nuclear Magnetic Resonance),EPR(Electron Paramagnetic Resonance),electrochemistry and DFT(Density Functional Theory).This multidisciplinary approach supports the presence of protons located on the organic ligands,and an electronic structure involving three high spin Ni_((II))ions strongly ferromagnetically coupled with radicals.Both ligand and complex provide a new design for molecular bricks and bioinspired energy storage devices.展开更多
基金support by the initiative of Excellence IDEX-Unistra(ANR-10-IDEX-0002-02)from the French National Program“Investment for the Future”,Agence Nationale pour la Recherche(ANR-20-CE05-0005-01,ANR-18-CE092-0040-01)CNRS and Universitéde StrasbourgLabex NIE(ANR-11-LABX-0058_NIE within the Investissement d’Avenir program)for the support to the magnetometry platform.
文摘We report the design of a unique bioinspired ligand merging redox-active catechol and flavin-related alloxazine substructures.Upon coordination with a Ni_((II))salt,this hybrid ligand forms a trinuclear complex containing three NiII centers and three redox-active ligands.This air-stable metallic triangle stabilizing protons and electrons was studied by X-ray crystallography,infra-red(IR)and UV-vis spectroscopy,SQUID magnetometry(Superconducting QUantum Interference Device),MAS-NMR(Magic Angle Spinning-Nuclear Magnetic Resonance),EPR(Electron Paramagnetic Resonance),electrochemistry and DFT(Density Functional Theory).This multidisciplinary approach supports the presence of protons located on the organic ligands,and an electronic structure involving three high spin Ni_((II))ions strongly ferromagnetically coupled with radicals.Both ligand and complex provide a new design for molecular bricks and bioinspired energy storage devices.
