Stabilization of a C2v‐Distorted Methane Derivative in an Organometallic Framework

An intramolecular ion-pair interaction stabilizes the unusual, distorted coordination geometry of C1 in 1. In the course of the topomerization 1⇋ent-1, which was followed by NMR spectroscopy, the internal Zr ⃛CH2 ion pair must be cleaved. The rearrangement pathway probably proceeds via a species with “normal” tetrahedral coordination geometry at C1.