Characterizing Gallium Dinitridocarbonates: A Focus on LiGa(CN ₂ ) ₂ , Li _13.6 Ga _2.8 (CN ₂ ) ₁₀ I ₂ , and SrGa ₂ (CN ₂ ) ₄

This study describes the synthesis and characterization of three new gallium dinitridocarbonates: LiGa(CN 2 ) 2 , Li 13.6 Ga 2.8 (CN 2 ) 10 I 2 , and SrGa 2 (CN 2 ) 4 . These compounds are obtained through solid‐state metathesis reactions, demonstrating an efficient route for the formation of dinitridocarbonate‐based materials. The crystal structures of LiGa(CN 2 ) 2 and Li 13.6 Ga 2.8 (CN 2 ) 10 I 2 are solved and refined in the orthorhombic space groups I 2 1 2 1 2 1 and Imma , respectively. The single‐crystal diffraction study of SrGa 2 (CN 2 ) 4 revealed the monoclinic space group P 2 1 /c . All the compounds under consideration feature networks based on metal‐centered tetrahedral arrangements. The presence of lithium in the compounds LiGa(CN 2 ) 2 and Li 13.6 Ga 2.8 (CN 2 ) 10 I 2 is confirmed by 7 Li magic‐angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy. Infrared spectroscopy measurements indicate the presence of carbodiimide and cyanamide units within the compounds. Furthermore, the optical reflectance of the air‐stable compound SrGa 2 (CN 2 ) 4 has shown to be a wide gap semiconductor.