Russian Chemical Bulletin p. 386 - 393 (1998)
Update date:2022-08-17
Topics:
Kazakov
Voloshin
Ostakhov
Zharinova
Catalysis of decomposition of dispiro(diadamantane-1,2-dioxetane) (1) in the presence of EuIII and TbIII tris(benzoyltrifluoroacetonate) complexes (Ln(btfa)3) accompanied by the formation of adamantanone (2) and chemiluminescence (CL) was studied. The rate constants (k2) of decomposition of compound 1 in the 1 · Ln(btfa)3 complexes and their stability constants (K1) have been determined. The Arrhenius parameters of decomposition of 1 (Ea = 22.4±0.7 kcal mol-1, logA = 10.2±0.8 for 1 · Tb(btfa)3 and Ea = 23.4±0.6 kcal mol-1, logA = 10.6±0.8 for 1 · Eu(btfa)3) and thermodynamic parameters of complex formation (ΔH = -5.5±0.5 kcal mol-1, ΔS = -10.4±0.7 e.u. for 1 · Tb(btfa)3 and ΔH = -5.8±0.5 kcal mol-1, ΔS = -10.9+0.7 e.u. for 1 · Eu(btfa)3) have been calculated from the temperature dependences of k2 and K1. The yields of excitation of the Ln(btfa)3 chelates φ*Eu = 0.021±0.006 and φ*Tb = 0.12±0.04 have been determined. A higher efficiency of the occupation of the 5D4-level of Tb3+ compared to those of the 5D1- and 5D0-levels of Eu3+ is caused by different efficiencies of the non-radiative energy dissipation in the Ln3+ ion after the intracomplex energy transfer from the 3n,π*-state of 2 to the resonance excited levels of lanthanides.
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