Sahoo, Rajata KumarRajata KumarSahooMukhopadhyay, SayantanSayantanMukhopadhyayRajput, SagrikaSagrikaRajputJana, AchintyaAchintyaJanaNembenna, SharanappaSharanappaNembenna2025-10-212025-10-212025-01-0110.1039/d4dt02907k2-s2.0-105018791608http://repository.iitgn.ac.in/handle/IITG2025/33329The tetra-aryl substituted bis-guanidine ligand L(3H) (L(3H) = {(ArHN)(ArNH)-CvN-C=(NAr)(NHAr)}, Ar = 2,6-ⁱPr<inf>2</inf>-C<inf>6</inf>H<inf>3</inf>) was used for the synthesis of mononuclear zinc(II) alkyl [L(2H)ZnR, R = Me (Zn-1), Et (Zn-2)], iodide [L(2H)ZnI, (Zn-3)], and hydride [L(2H)ZnH, (Zn-4)] complexes. Moreover, the reactions of Zn-1, Zn-2, and Zn-3 with [PhNMe<inf>2</inf>H]⁺ [B(C<inf>6</inf>F<inf>5</inf>)<inf>4</inf>]⁻ yielded the biguanide zinc alkyl [L(3H)ZnR]⁺ [B(C<inf>6</inf>F<inf>5</inf>)<inf>4</inf>]⁻ (R = Me (Zn-5), Et (Zn-6)) and iodide [L(3H)ZnI]⁺ [B(C<inf>6</inf>F<inf>5</inf>)<inf>4</inf>]⁻ (Zn-7) cationic compounds in good yields. All newly isolated and thermally stable zinc complexes (Zn-1-Zn-7) were well characterized by multinuclear NMR (¹H, ¹³C{¹H}, with additional ¹¹B and ¹⁹F{¹H} for Zn-5-Zn-7), HRMS, and single crystal X-ray diffraction studies. Moreover, the well-defined zinc iodide cation (Zn-7) [L(3H)ZnI]⁺ [B(C<inf>6</inf>F<inf>5</inf>)<inf>4</inf>]⁻ was further used as a catalyst for the synthesis of cyanohydrin enol ether products (RCR’CNOSiMe<inf>3</inf>) by TMSCN addition to carbonyl compounds (RCOR’, R’ = alkyl/aryl) under mild reaction conditions.trueArticlehttps://pubs.rsc.org/en/content/articlepdf/2025/dt/d4dt02907k14779234202500WOS:001582939900001