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Gas-phase observation and CO substitution kinetics of cis-Cr(CO)/sub 4/(C/sub 2/H/sub 4/)/sub 2/ by time-resolved IR absorption spectrometry

Journal Article · · J. Am. Chem. Soc.; (United States)
DOI:https://doi.org/10.1021/ja00238a049· OSTI ID:6970513

Olefin complexes of metal carbonyl fragments have theoretical importance and play a role in numerous catalytic systems. Theory suggests an interesting trend in bond strengths for the bis-olefin and diene complexes of the 16-electron group VI (group 6) carbonyl fragments. Bis-olefin complexes of M(CO)/sub 4/ (M = Cr, Mo, W) are generally thought to be more stable than eta/sup 4/-diene complexes. Experiments show that the mono- and bis-olefin complexes of molybdenum and tungsten carbonyls are quite stable but such examples for chromium are rare. Only one Cr(CO)/sub 4/(olefin)/sub 2/ complex is known and it is stabilized by relief of ring strain in the uncomplexed olefin. Interestingly, the analogous eta/sup 4/ complexes of nonconjugated dienes are generally quite stable for all three rows of group VI (group 6). This paper reports the first gas-phase observation and infrared spectral characterization of Cr(CO)/sub 4/(C/sub 2/H/sub 4/)/sub 2/. This complex is unstable and reacts with CO by dissociative substitution. They follow the kinetics of this process by time-resolved IR absorption spectrometry, extracting a unimolecular decay constant orders of magnitude larger than the reported solution value for Cr-(CO)/sub 4/(eta/sup 4/-butadiene), in an apparent conflict with elementary theory as cited above.

Research Organization:
Purdue Univ., West Lafayette, IN
OSTI ID:
6970513
Journal Information:
J. Am. Chem. Soc.; (United States), Journal Name: J. Am. Chem. Soc.; (United States) Vol. 109:4; ISSN JACSA
Country of Publication:
United States
Language:
English