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/sup 59/Co NMR of cobalt(III) porphyrin complexes. 2. Electric field gradients, d-orbital populations, and hydrogen bonding

Journal Article · · J. Am. Chem. Soc.; (United States)
DOI:https://doi.org/10.1021/ja00229a014· OSTI ID:6048065
A series of six-coordinate cobalt(III) tetraphenylporphyrin complexes with para substituents on the phenyl groups and with a variety of axial imidazole ligands has been prepared. The /sup 59/Co NMR spectra of these complexes in a number of solvents and at several field strengths are reported. Shielding anisotropy is very small, confirming the authors earlier suggestion that porphyrin, imidazole, and ammonia ligands have nearly the same position in the spectrochemical series. The chemical shift /delta/ and line width /omega//sub 1/2/ increase as the para substituent on the TPP phenyl rings becomes electron-releasing. Correlations of /delta/ and /omega//sub 1/2/ with Hammett /sigma/ substituent constants are noted. A simple molecular orbital model is used to rationalize both chemical shift and line width changes. It is concluded that variations in /omega//sub 1/2/ with substituent arise from changes in the electric field gradient, q, which in turn depends on the extent of mixing of metal 3d and ligand /pi/ orbitals. The chemical shift and line width also depend on the substituent on the imidazole N-1 nitrogen. In particular, hydrogen bonding to solvent or added base from axial imidazoles containing N-H group strongly affects /omega//sub 1/2/, and the conclusion is reached that /sup 59/Co NMR is a good way to study such proximal hydrogen-bonding interactions. The /sup 59/Co NMR spectra are dominated by quadrupolar relaxation, and this is discussed along with other possible relaxation mechanisms. 61 references, 7 figures, 5 tables.
Research Organization:
Brown Univ., Providence, RI (USA)
OSTI ID:
6048065
Journal Information:
J. Am. Chem. Soc.; (United States), Journal Name: J. Am. Chem. Soc.; (United States) Vol. 110:21; ISSN JACSA
Country of Publication:
United States
Language:
English