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Kinetics of acetyl radical formation from methyl radicals and carbon monoxide and crystal structures of two acetylcobalt complexes

Journal Article · · Inorganic Chemistry; (United States)
DOI:https://doi.org/10.1021/ic00050a011· OSTI ID:6827129

Methyl radicals react with macrocyclic cobalt complexes (H[sub 2]O)[sub 2]LCo[sup 2+] (L[sup 1] = 1,4,8,11-tetraazacyclotetradecane, L[sup 2] = C-meso-5,7,7,12,14,14-hexamethyl-1,4,8,11-tetraazacyclotetradecane) in the presence of CO in acidic aqueous solution. The reaction yields a mixture of methyl and acetyl complexes as a result of the competition between CO and (H[sub 2]O)[sub 2]CoL[sup 2+] for CH[sub 3][center dot]. Kinetic competition experiments yielded the rate constant for the capture of CH[sub 3][center dot] by CO, k[sub CO] = (2.0 [+-] 0.3) [times] 10[sup 6] M[sup [minus]1] s[sup [minus]1]. The acetyl complex of CoL[sup 1] crystallizes with either H[sub 2]O or ClO[sub 4][sup [minus]] coordinated trans to the acetyl group. Both the red [(ClO[sub 4])L[sup 1]CoC(O)CH[sub 3]](ClO[sub 4]) (1) and the yellow [(H[sub 2]O)L[sup 1]-CoC(O)CH[sub 3]](ClO[sub 4])[sub 2][center dot]H[sub 2]O (2) crystallize in the centric space group P2[sub 1]/c with four molecules in a unit cell of dimensions a = 10.539 (1) [angstrom], b = 12.548 (2) [angstrom], c = 14.915 (2) [angstrom], and [beta] = 93.74 (3)[degree] for 1 and a = 12.588 (3) [angstrom], b = 8.821 (3) [angstrom], c = 19.398 (5) [angstrom], and [beta] = 96.34 (2)[degree] for 2. The data refined to final values of the unweighted R factors of 0.037 (1) and 0.054 (2).

DOE Contract Number:
W-7405-ENG-82
OSTI ID:
6827129
Journal Information:
Inorganic Chemistry; (United States), Journal Name: Inorganic Chemistry; (United States) Vol. 31:24; ISSN 0020-1669; ISSN INOCAJ
Country of Publication:
United States
Language:
English