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Models of dithiolate rhenium(V)–oxo and –thio complexes and ReVII (ReVIIO2 and ReVIIOS) intermediates are studied computationally using DFT(B3LYP). The analysis of the Re–E bond (E = O, S) shows that the two lone pairs (Px, Py) on the oxo and thio ligands are strongly polarized to the ReV and ReVII centers, forming partial π bonds, which agree with the bond‐order analysis of 2 (one σ + two partial...
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