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Mereshchenko, Andrey S; Olshin, Pavel K; Karabaeva, Kanykey E; Panov, Maxim S; Wilson, R. Marshall; Kochemirovsky, Vladimir A; Skripkin, Mikhail Yu; Tveryanovich, Yury S; Tarnovsky, Alexander N
The journal of physical chemistry. B, 07/2015, Letnik: 119, Številka: 28Journal Article
Copper(II) complexes are extremely labile with typical ligand exchange rate constants on the order of 106–109 M–1 s–1. As a result, it is often difficult to identify the actual formation mechanism of these complexes. In this work, using UV–vis transient absorption when probing in a broad time range (20 ps to 8 μs) in conjunction with DFT/TDDFT calculations, we studied the dynamics and underlying reaction mechanisms of the formation of extremely labile copper(II) CuCl4 2– chloro complexes from copper(II) CuCl3 – trichloro complexes and chloride ions. These two species, produced via photochemical dissociation of CuCl4 2– upon 420 nm excitation into the ligand-to-metal-charge-transfer electronic state, are found to recombine into parent complexes with bimolecular rate constants of (9.0 ± 0.1) × 107 and (5.3 ± 0.4) × 108 M–1 s–1 in acetonitrile and dichloromethane, respectively. In dichloromethane, recombination occurs via a simple one-step addition. In acetonitrile, where CuCl3− reacts with the solvent to form a CuCl3CH3CN− complex in less than 20 ps, recombination takes place via ligand exchange described by the associative interchange mechanism that involves a CuCl4CH3CN2– intermediate. In both solvents, the recombination reaction is potential energy controlled.
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