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• W2010054082 abstract "The rate coefficients and product ion distributions have been determined at 80, 205, and 295 K for the reactions of CH3+, CH2D+, CHD2+, and CD3+ with H2, HD, and D2 using a SIFT apparatus. Two types of reactions were observed, those involving isotope (H/D) exchange and those in which ion–molecule collisionally stabilized association occurs. Both exoergic and endoergic isotope exchange occurred and often more than one product was observed. Example reactions are (1) CH3++HD⇄CH2D++H2, (2) CD3++H2→CHD2++HD, CH2D++D2,CH2D3+. The exchange reactions are exoergic when H atoms in the reactant ion are exchanged for D atoms from the reactant neutral. As expected, the reverse (endoergic) rate coefficients kr decrease with decreasing temperature, whereas the forward (exoergic) rate coefficients kf increase with decreasing temperature. From the kf and kr for some of these reactions van’t Hoff plots have been constructed and thus ΔH° and ΔS° have been obtained. Using the experimentally determined values for ΔH°, the difference in the strengths of the C–H and C–D bonds in CH3+ like ions has been determined to be 1.56 kcal mol−1. Only collisional association can be observed in the CH3++H2 and CD3+ +D2 reactions. In several reactions, however, association is observed to compete with endoergic isotope exchange and at 80 K it is the dominant channel in reactions such as (2). At 80 K the ternary association rate coefficient k3 is smallest for the CH3++H2 reaction and largest for the CD3++H2 reaction (rather than the CD3++D2 reaction). This is tentatively explained not only in terms of the increased densities of states in the deuterated intermediate complexes which increase their lifetimes against unimolecular decomposition (and hence increase k3), but also to ’’isotopic refrigeration’’ which results from the rearrangement of H and D atoms in the CH5+ like complexes." @default.
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• W2010054082 date "1982-08-01" @default.
• W2010054082 modified "2023-10-14" @default.
• W2010054082 title "Isotope exchange and collisional association in the reactions of CH3+ and its deuterated analogs with H2, HD, and D2" @default.
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• W2010054082 doi "https://doi.org/10.1063/1.444002" @default.
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