Reactivity of CnHx+ (n=24, 18; x=0-12) cluster ions toward benzene

Guo X, Grützmacher H-F (1999)
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 121(18): 4485-4494.

Zeitschriftenaufsatz | Veröffentlicht | Englisch
 
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Abstract / Bemerkung
C-24(.+) carbon cluster ions as well as C24Hx+ and C18Hx+ cluster ions of low hydrogen content were produced in a FT-ICR spectrometer by repeated losses of H-. atoms from the molecular ions of coronene C24H12 and of the 4 isomeric polycyclic aromatic hydrocarbons (PAH) C18H12 triphenylene, chrysene, 1,2-benzanthracene, and 2,3-benzanthracene, respectively, using a sequence of SORI-CID procedures. Then, the selected cluster ions were reacted with benzene and benzene-d(6) to yield product ions [CnHx. nC(6)H(6)](+), n = 1-3, and [CnHx-1. nC(6)H(6)](+). In the latter case it was proven by reaction with C6D6 that the H-. atom lost originates exclusively from the CnHx part of the original cluster ions. In most cases, bimodal kinetics were observed due to a fraction of cluster ions with low or no reactivity toward benzene. The bimolecular rate constants k(bi) of the reactions of all reactive cluster ions were determined. For C24Hx+ ions the C24H12.+ molecular ions of coronene and the C24H10.+ ions do not undergo a reaction with benzene, while for the other C24Hx+ ions the rate constants increase with decreasing number x of H-. atoms but exhibit an odd/even alternation. The even-electron C24H2m+1+ cations are generally more reactive than the C24H2m.+ odd-electron radical cations. The rate constant of the reaction of benzene with the C-24(.+) carbon cluster ion eventually produced by SORI-CID from coronene exceeds the rate constant of the same reaction of monocyclic C-24(.+) carbon cluster ion generated by laser evaporation of graphite by more than 3 orders of magnitude. This shows unambiguously that C-24(.+) cluster ions of a different structure are generated by the SORI-CID technique. It is suggested that these C-24(.+) ions retain the graphitic structure of the precursor coronene. This is corroborated by the study of 4 series of C18Hx+ ions derived from the 3 isomeric PAHs. These ions exhibit analogous and as characteristic reactions with benzene as the C24Hx+ ions, but the rate constants of individual C18Hx+ ions are different for the 4 isomeric precursor PAHs. This indicates very strongly that all these CnHx+ ions produced by repeated losses of H-. atoms from ionized PAHs with a sequence of SORI-CID procedures retain the graphitic structures of the precursor molecules.
Erscheinungsjahr
1999
Zeitschriftentitel
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Band
121
Ausgabe
18
Seite(n)
4485-4494
ISSN
0002-7863
eISSN
1520-5126
Page URI
https://pub.uni-bielefeld.de/record/1622963

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Guo X, Grützmacher H-F. Reactivity of CnHx+ (n=24, 18; x=0-12) cluster ions toward benzene. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY. 1999;121(18):4485-4494.
Guo, X., & Grützmacher, H. - F. (1999). Reactivity of CnHx+ (n=24, 18; x=0-12) cluster ions toward benzene. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 121(18), 4485-4494. https://doi.org/10.1021/ja984275e
Guo, Xinghua, and Grützmacher, Hans-Friedrich. 1999. “Reactivity of CnHx+ (n=24, 18; x=0-12) cluster ions toward benzene”. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 121 (18): 4485-4494.
Guo, X., and Grützmacher, H. - F. (1999). Reactivity of CnHx+ (n=24, 18; x=0-12) cluster ions toward benzene. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 121, 4485-4494.
Guo, X., & Grützmacher, H.-F., 1999. Reactivity of CnHx+ (n=24, 18; x=0-12) cluster ions toward benzene. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 121(18), p 4485-4494.
X. Guo and H.-F. Grützmacher, “Reactivity of CnHx+ (n=24, 18; x=0-12) cluster ions toward benzene”, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, vol. 121, 1999, pp. 4485-4494.
Guo, X., Grützmacher, H.-F.: Reactivity of CnHx+ (n=24, 18; x=0-12) cluster ions toward benzene. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY. 121, 4485-4494 (1999).
Guo, Xinghua, and Grützmacher, Hans-Friedrich. “Reactivity of CnHx+ (n=24, 18; x=0-12) cluster ions toward benzene”. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 121.18 (1999): 4485-4494.
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