Journal of the American Chemical Society p. 4124 - 4128 (1982)
Update date:2022-08-30
Topics:
Mulac, William A.
Meyerstein, Dan
The spectra of the intermediates formed in the reactions of B12r with the free radicals Br2-*, CO2-*, *CH2C(CH3)2OH, *C(CH3)2OH, *CH2CHO, and *CH(OH)CH2OH are reported.The results indicate that Br2-* oxidizes B12r to B12a, via an inner-sphere mechanism, and CO2-* reduces B12r to B12s.All the aliphatic free radicals studied, *R, react with B12r, yielding as the first product a pseudocoenzyme denoted CoIII-R.CoIII-CH2C(CH3)2OH is stable for over a second in the pH range 3-10 as is CoIII-CH2CHO.The latter compound hydrolyzes in acid solutions to yield B12a and CH3CHO.CoIII-C(CH3)2OH and COIII-CH(OH)CH2OH decompose heterolytically to yield mainly B12s; a side reaction that probably yields CoIII-H via a β-hydride shift is also observed.The kinetics of decomposition of CoIII-CH(OH)CH2OH in neutral solutions are reported.No water elimination from the latter intermediate occurs.The reasons for the latter observation are discussed.
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