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Baykov, Sergey V; Katlenok, Eugene A; Baykova, Svetlana O; Semenov, Artem V; Bokach, Nadezhda A; Boyarskiy, Vadim P
International journal of molecular sciences, 04/2024, Letnik: 25, Številka: 7Journal Article
The nucleophilic addition of 3-(4-cyanopyridin-2-yl)-1,1-dimethylurea (1) to cis-Pt(CNXyl)sub.2Clsub.2 (2) gave a new cyclometallated compound 3. It was characterized by NMR spectroscopy (sup.1H, sup.13C, sup.195Pt) and high-resolution mass spectrometry, as well as crystallized to obtain two crystalline forms (3 and 3·2MeCN), whose structures were determined by X-ray diffraction. In the crystalline structure of 3, two conformers (3A and 3B) were identified, while the structure 3·2MeCN had only one conformer 3A. The conformers differed by orientation of the N,N-dimethylcarbamoyl moiety relative to the metallacycle plane. In both crystals 3 and 3·2MeCN, the molecules of the Pt(II) complex are associated into supramolecular dimers, either {3A}sub.2 or {3B}sub.2, via stacking interactions between the planes of two metal centers, which are additionally supported by hydrogen bonding. The theoretical consideration, utilizing a number of computational approaches, demonstrates that the C···dzsup.2(Pt) interaction makes a significant contribution in the total stacking forces in the geometrically optimized dimer 3Asub.2 and reveals the dsub.z sup.2(Pt)→π*(PyCN) charge transfer (CT). The presence of such CT process allowed for marking the C···Pt contact as a new example of a rare studied phenomenon, namely, tetrel bonding, in which the metal site acts as a Lewis base (an acceptor of noncovalent interaction).
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