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Mechanism of the formation of cationic species in the radiolysis of butyl chlorides. I. [2. 7-2. 8 MeV electron pulses; n- and sec-butyl chlorides]

Journal Article · · J. Phys. Chem.; (United States)
DOI:https://doi.org/10.1021/j100559a003· OSTI ID:7353295

Radiation chemical studies were carried out on n- and sec-butyl chlorides using low-temperature pulse radiolysis and matrix isolation techniques. The pulse radiolysis of n-butyl chloride at 133/sup 0/K yields the same absorption spectrum as observed for ..gamma..-irradiated n-butyl chloride at 77/sup 0/K. The initial spectrum has a peak at 520 nm, however, the peak shifts to 450 nm within 80 ..mu..s. The absorption decay behavior indicated that the initial spectrum is due to a long-lived species with a peak at 450 nm as well as a short-lived species with a peak at about 550 nm. The effects of additives on both species suggest that the long- and short-lived species are butene cations and n-butyl chloride cations, respectively. The spectra of butene-1, cis-butene-2, and trans-butene-2 cations obtained using a matrix isolation technique also show peaks in the vicinity of 450 nm. In a solution of 0.031 mole percent biphenyl at 133/sup 0/K, a significant amount of biphenyl cations is produced simultaneously with pulse irradiation, although they are also produced slowly by charge transfer between biphenyl molecules and n-butyl chloride and butene cations. Addition of biphenyl to n-butyl chloride at 77/sup 0/K reduces the formation of both butene and n-butyl chloride cations by the same ratio, and is accompanied by the formation of biphenyl cations. Therefore, butene and n-butyl chloride cations must originate from a common precursor, which reacts with biphenyl forming its cation. The nature of the precursor is discussed on the basis of the observed results. It is probably a vibrationally excited n-butyl chloride cation. Radiolysis of sec-butyl chloride gives results similar to n-butyl chloride.

Research Organization:
Inst. of Physical and Chemical Research, Saitama, Japan
OSTI ID:
7353295
Journal Information:
J. Phys. Chem.; (United States), Journal Name: J. Phys. Chem.; (United States) Vol. 80:18; ISSN JPCHA
Country of Publication:
United States
Language:
English