Abstract
Polydentate complexes containing combinations of nitrogen and carbon (N and C) ligating atoms are among the most fundamental and ubiquitous molecules in coordination chemistry, yet the formation of such complexes with planar high-coordinate N/C sites remains challenging. Herein, we demonstrate an efficient route to access related complexes with tetradentate CCCN and pentadentate CCCCN and NCCCN cores by successive modification of the coordinating atoms in complexes with a CCCC core. Combined experimental and computational studies reveal that the rich reactivity of metal-carbon bonds and the inherent aromaticity of the metallacyclic skeletons play key roles in these transformations. This strategy addresses the paucity of synthetic approaches to mixed N/C planar pentadentate chelating species and provides valuable insights into the synthesis of carbon-based high-coordinate complexes. Furthermore, the resulting complexes are the examples of organometallic species with combined photoacoustic, photothermal, and sonodynamic properties, which makes them promising for application in related areas.
Highlights
Polydentate complexes containing combinations of nitrogen and carbon (N and C) ligating atoms are among the most fundamental and ubiquitous molecules in coordination chemistry, yet the formation of such complexes with planar high-coordinate N/C sites remains challenging
Carbon can serve as a coordinating atom in a polydentate complex, and it usually appears in combination with other classical donor atoms[5,6]; such complexes have been theoretically and experimentally examined due to their unique structural, electronic, aromatic, catalytic, and optical properties[7,8,9,10]
The chemistry of molecules with higher planar carbon/nitrogen (C/N) coordination sites, such as those allowing penta- and hexacoordination, remains unexplored owing to the inaccessibility of the atypical geometries, especially for the complexes based on transition metal centers
Summary
Polydentate complexes containing combinations of nitrogen and carbon (N and C) ligating atoms are among the most fundamental and ubiquitous molecules in coordination chemistry, yet the formation of such complexes with planar high-coordinate N/C sites remains challenging. We report the successive transformation of the coordinating atoms in complex with a CCCC core, which can undergo unique changes in molecular topology, such as a shift of the aromatic unit.
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