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Emil Mickey Hilligsøe Larsen1, Theis Brock-Nannestad1, Jørgen Skibsted2

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This study presents the first homoleptic silver(III) complex with N-donor ligands. The novel argentate(III) ion, [Ag(succ)4]-, was synthesized and characterized, showing unique electronic properties and reactivity.

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Area of Science:

  • Inorganic Chemistry
  • Coordination Chemistry
  • Materials Science

Background:

  • Silver(I) complexes are common, but higher oxidation states like silver(III) are less explored.
  • Homoleptic complexes, where all ligands are identical, offer simplified systems for studying metal ion properties.
  • N-donor ligands are crucial in stabilizing metal ions in various oxidation states.

Purpose of the Study:

  • To synthesize and characterize the first homoleptic silver(III) complex stabilized by a monodentate N-donor ligand.
  • To investigate the electronic structure and properties of the novel silver(III) complex.
  • To explore the reactivity of the silver(III) complex, particularly its potential in oxidation reactions.

Main Methods:

  • Oxidation of a linear silver(I) complex (Na[Ag(succ)2]) using sodium persulfate (Na2S2O8).
  • Crystallization with alkali metal sulfates to form polymeric chain structures (M[Ag(succ)4]).
  • Spectroscopic characterization including UV-vis spectroscopy and 109Ag magic-angle spinning NMR.
  • Comparison with an isoelectronic palladium(II) complex for electronic property analysis.

Main Results:

  • Formation of a square planar argentate(III) ion, [Ag(succ)4]-, stabilized by succinimide ligands.
  • Crystallization into polymeric chain structures (M[Ag(succ)4]) and a mixed-valent system (2^Ag).
  • Diamagnetic 2^Cs showed higher energy C=O stretching and more intense, lower energy UV-vis absorptions compared to the Pd(II) analog.
  • The electron-deficient Ag(III) complex demonstrated the ability to oxidize water to O2.
  • 109Ag NMR revealed a highly deshielded Ag(III) environment (2080 ppm) compared to Ag(I) (492 ppm).

Conclusions:

  • The successful synthesis of a homoleptic Ag(III) complex with N-donor ligands opens new avenues in silver chemistry.
  • The characterized argentate(III) complex exhibits unique electronic and redox properties, including water oxidation capability.
  • This work provides valuable insights into the coordination chemistry and reactivity of silver in its +3 oxidation state.