Direct evidence for chemically distinct regions within nation films on electrodes |
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| Institution: | 1. Facultad de Ciencias Químicas, Universidad Veracruzana, Prolongación de Oriente 6, No. 1009, Col. Rafael Alvarado, C.P. 94340, Orizaba, Veracruz, Mexico;2. Departamento de Ecomateriales y Energía, Facultad de Ingeniería Civil, Universidad Autónoma de Nuevo León, Av. Universidad S/N, Ciudad Universitaria, C.P. 64455, San Nicolás de los Garza, Nuevo León, Mexico;3. Instituto de Química, Universidad Nacional Autónoma de México, Circuito Exterior S/N, C.P. 04510, Ciudad de México, Mexico;1. Department of Chemistry, Inter-departmental Center NIS and INSTM, University of Turin, Via Pietro Giuria 7, 10125 Torino, Italy;2. Univ Paris Est Creteil, CNRS, ICMPE, UMR 7182, 2 rue Henri Dunant, 94320 Thiais, France;3. Institute of Hydrogen Technology, Helmholtz-Zentrum Hereon, Max-Planck-Straße 1, 21502 Geesthacht, Germany;4. Department for Hydrogen Technology, Institute for Energy Technology, P.O. Box 40, Kjeller NO-2027, Norway;1. Département de Chimie, Centre de Catalyse et Chimie Verte (C3V), Université Laval, 1045 Avenue de la Médecine, Québec, Québec G1V 0A6, Canada;2. Department of Chemistry, University of Toronto, 80 St. George St., Toronto, Ontario M5S 3H6, Canada |
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| Abstract: | Electrochemical and spectroelectrochemical experiments on the complexes (bpy)2(py)RuII(OH2)]2+ and (trpy)(bpy)RuII(OH2)]2+ (py is pyridine; bpy is 2,2'-bipyridine; trpy is 2,2',2“-terpyridine) with Nation films coated on electrodes demonstrate that the complexes partition amongst three chemically distinct regions or phases. As Ru(II) the complexes reside both in an electroinactive phase and, based on the pH dependence of the Ru(III)/(II) couples, e.g., (bpy)2(py)RuIII(OH)]2+/(bpy)2(py)RuII(OH2)]2+, in two electroactive phases. Partitioning amongst the three phases depends on the pH of the external solution and on the oxidation state and proton content of the complex. Addition of alcohols releases the complex from the electroinactive phase but at the expense of loss of the bound water molecule and binding to the sulfonate sites by anation and, therefore, to a fourth distinct chemical or physical state in which the complex can exist within Nation films. |
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