Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases p. 2467 - 2478 (1982)
Update date:2022-08-28
Topics:
Solar, Sonja
Solar, Wolfgang
Getoff, Nikola
Holcman, Jerzy
Sehested, Knud
Pulse radiolysis of air-free aqueous methyl viologen (MV2+) solutions was carried out at various pH.The attack of e-aq on MV2+, with k(e-aq + MV2+) = 7.5*1010 dm3 mol-1 s-1, leads to the formation of the long-lived radical cation (MV.+), which possesses two absorption maxima at 392.5 nm (ε392.5 = 4200 m2 mol-1) and 600 nm (ε600 = 1450 m2 mol-1).The H-atoms react with MV2+ at pH 1 forming two species, which have superimposed absorption bands.By means of a computer simulation they are resolved in the absorptions belonging to: (1) a protonated form of the radical cation (MV.+H+), which is produced with k(H + MV2+) = (3.5+/-0.2)*108 dm3 mol-1 s-1, has 2 absorption maxima at 390 nm (ε390 = 1700 m2 mol-1) and 595 nm (ε595 = 760 m2 mol-1) and decays by second-order kinetics with k = 3.5*109 dm3 mol-1 s-1; (2) an H-adduct (MV.2+H) on the ring carbon, which is formed with k(H + MV2+) = 2.5*108 dm3 mol-1 s-1, absorbs at 310 nm (ε310 = 900 m2 mol-1) and 470 nm (ε470 = 630 m2 mol-1) and decays by conversion into MV.+H+ in a first-order process with k = 6*103 s-1.For the equilibrium MV.+H+ <*> MV.+ + H+ pK = 2.9+/-0.1 was determined.The presented data explain, at least partly, the instability of MV2+ when used as an electron acceptor in various devices for utilization of solar energy.
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(1983)
