5 years ago

Following a Chemical Reaction on the Millisecond Time Scale by Simultaneous X-ray and UV/Vis Spectroscopy

Following a Chemical Reaction on the Millisecond Time Scale by Simultaneous X-ray and UV/Vis Spectroscopy
Giorgio Olivo, Osvaldo Lanzalunga, Theyencheri Narayanan, Paola D’Angelo, Sakura Pascarelli, Manuel Monte, Valeria Dantignana, Alessia Barbieri, Stefano Di Stefano, Valentina Migliorati, Francesco Sessa
An innovative approach aimed at disclosing the mechanism of chemical reactions occurring in solution on the millisecond time scale is presented. Time-resolved energy dispersive X-ray absorption and UV/vis spectroscopies with millisecond resolution are used simultaneously to directly follow the evolution of both the oxidation state and the local structure of the metal center in an iron complex. Two redox reactions are studied, the former involving the transformation of FeII into two subsequent FeIII species and the latter involving the more complex FeII–FeIII–FeIV–FeIII sequence. The structural modifications occurring around the iron center are correlated to the reaction mechanisms. This combined approach has the potential to provide unique insights into reaction mechanisms in the liquid phase and represents a new powerful tool to characterize short-lived intermediates that are silent to common spectroscopic techniques.

Publisher URL: http://dx.doi.org/10.1021/acs.jpclett.7b01133

DOI: 10.1021/acs.jpclett.7b01133

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