Abstract
The nature of the interaction between chloromethanes CH4–nClnand Pt(II) complexes has been studied by high‐pressure X‐ray diffraction and infrared spectroscopy in combination with DFT calculations. In case of electron rich complexes such as d8‐Pt(btz‐N,N′)(phenyl)LwithL= phenyl, Cl, Br and btz = 2,2′‐Bi‐5,6‐dihydro‐4H‐1,3‐thiazine stable chloroform adducts with bridging hydrogen atoms in the η1(C–H)Pt moieties were isolated which display highly activated C–H bonds. This activation is a consequence of a pronounced Pt(dz²)→σ*(C–H) back donation and is signaled by large red‐shifts of the isolatedνis(C–H) stretching modes. The extent of the C–H bond activation and covalent Pt–H bond formation in the η1(C–H)Pt moieties is thereby controlled by (i) the σ/π donor capabilities of the ligandsL, (ii) the orientation of the coordinating C–H bond with regard to the Pt(dz²) orbital and (iii) the applied pressure.
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