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      Graphene nanoreactors : photoreduction of prussian blue in aqueous solution

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      Author(s)
      Nappini, Silvia
      Matruglio, Alessia
      Naumenko, Denys
      Dal Zilio, Simone
      Lazzarino, Marco
      De Groot, Frank M.F.
      Kocabaş, Coşkun
      Balcı, Osman
      Magnano, Elena
      Date
      2017
      Source Title
      Journal of Physical Chemistry C
      Print ISSN
      1932-7447
      Publisher
      American Chemical Society
      Volume
      121
      Issue
      40
      Pages
      22225 - 22233
      Language
      English
      Type
      Article
      Item Usage Stats
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      Abstract
      Prussian dyes are characterized by interesting photomagnetic properties due to the photoinduced electron transfer involved in the Fe oxidation and spin state changes. Ferromagnetic Prussian blue (PB) in contact with titanium dioxide (TiO2) can be reduced to paramagnetic Prussian white (PW) upon UV band gap excitation of TiO2. This process is promoted by the presence of a hole scavenger, such as water, fundamental to ensure the overall charge balance and the continuity of the process. In order to clarify the photoinduced reduction mechanism and the role of water, an innovative system of graphene nanobubbles (GNBs) filled with a PB aqueous solution was developed, enabling the application of electron spectroscopies to the liquid phase, up to now limited by the vacuum required to overcome the short electron inelastic mean free path in dense medium. In this work GNBs formed on the photocatalytic substrate are able to act as "nanoreactors", and they can control and take part in the reaction. The evolution of Fe L2,3 edge X-ray absorption spectra measured in total electron yield through the graphene membrane revealed the electron reduction from PB (FeIII-CN-FeII) to PW (FeII-CN-FeII) upon UV irradiation, shedding light on the photoinduced electron transfer mechanism in liquid phase. The results, confirmed also by Raman spectroscopy, unequivocally demonstrate that the reaction occurs preferentially in aqueous solution, where water acts as hole scavenger.
      Keywords
      Redox reactions
      Oxides
      Photoinduced electrons
      Solution chemistry
      Irradiation
      Permalink
      http://hdl.handle.net/11693/37295
      Published Version (Please cite this version)
      http://dx.doi.org/10.1021/acs.jpcc.7b07898
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