Surface Protonation and Electrochemical Activity of Oxides in Aqueous Solution

J. B. Goodenough; R. Manoharan; M. Paranthaman

doi:10.1021/ja00162a006

Surface Protonation and Electrochemical Activity of Oxides in Aqueous Solution

J. B. Goodenough, R. Manoharan, M. Paranthaman

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Abstract

Measurements of the pH dependence of the surface-charge density on oxide particles are correlated with the pHdependence of the cyclic voltammograms and of the chemical activity of the oxide for electrolysis/fuel cell reactions. Studies of the pyrochlores Pb₂M_2-xPb_xO_7-y and the rutiles MO₂ (M = Ru or Ir) and of the perovskite Sr_1-xNbO_3-δ show that (1) the oxygen-reduction reaction, found on the pyrochlores in alkaline solution, occurs by exchange of a surface OH^- species at anO' site with an adsorbed O₂^- solution species, (2) the oxygen-evolution and chlorine-evolution reactions occur at a surfaceO^- species made accessible by surface oxidation of a redox couple lying close to the top of the O^2-:2p⁶ valence band, and (3)the hydrogen-evolution reaction occurs at the surface OH₂ species bonded to cations with a surface redox couple lying close to the H⁺H level in solution.

Original language	English
Pages (from-to)	2076-2082
Number of pages	7
Journal	Journal of the American Chemical Society
Volume	112
Issue number	6
DOIs	https://doi.org/10.1021/ja00162a006
State	Published - Jan 1990
Externally published	Yes

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title = "Surface Protonation and Electrochemical Activity of Oxides in Aqueous Solution",

abstract = "Measurements of the pH dependence of the surface-charge density on oxide particles are correlated with the pHdependence of the cyclic voltammograms and of the chemical activity of the oxide for electrolysis/fuel cell reactions. Studies of the pyrochlores Pb2M2-xPbxO7-y and the rutiles MO2 (M = Ru or Ir) and of the perovskite Sr1-xNbO3-δ show that (1) the oxygen-reduction reaction, found on the pyrochlores in alkaline solution, occurs by exchange of a surface OH- species at anO' site with an adsorbed O2- solution species, (2) the oxygen-evolution and chlorine-evolution reactions occur at a surfaceO- species made accessible by surface oxidation of a redox couple lying close to the top of the O2-:2p6 valence band, and (3)the hydrogen-evolution reaction occurs at the surface OH2 species bonded to cations with a surface redox couple lying close to the H+H level in solution.",

author = "Goodenough, {J. B.} and R. Manoharan and M. Paranthaman",

year = "1990",

month = jan,

doi = "10.1021/ja00162a006",

language = "English",

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journal = "Journal of the American Chemical Society",

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TY - JOUR

T1 - Surface Protonation and Electrochemical Activity of Oxides in Aqueous Solution

AU - Goodenough, J. B.

AU - Manoharan, R.

AU - Paranthaman, M.

PY - 1990/1

Y1 - 1990/1

N2 - Measurements of the pH dependence of the surface-charge density on oxide particles are correlated with the pHdependence of the cyclic voltammograms and of the chemical activity of the oxide for electrolysis/fuel cell reactions. Studies of the pyrochlores Pb2M2-xPbxO7-y and the rutiles MO2 (M = Ru or Ir) and of the perovskite Sr1-xNbO3-δ show that (1) the oxygen-reduction reaction, found on the pyrochlores in alkaline solution, occurs by exchange of a surface OH- species at anO' site with an adsorbed O2- solution species, (2) the oxygen-evolution and chlorine-evolution reactions occur at a surfaceO- species made accessible by surface oxidation of a redox couple lying close to the top of the O2-:2p6 valence band, and (3)the hydrogen-evolution reaction occurs at the surface OH2 species bonded to cations with a surface redox couple lying close to the H+H level in solution.

AB - Measurements of the pH dependence of the surface-charge density on oxide particles are correlated with the pHdependence of the cyclic voltammograms and of the chemical activity of the oxide for electrolysis/fuel cell reactions. Studies of the pyrochlores Pb2M2-xPbxO7-y and the rutiles MO2 (M = Ru or Ir) and of the perovskite Sr1-xNbO3-δ show that (1) the oxygen-reduction reaction, found on the pyrochlores in alkaline solution, occurs by exchange of a surface OH- species at anO' site with an adsorbed O2- solution species, (2) the oxygen-evolution and chlorine-evolution reactions occur at a surfaceO- species made accessible by surface oxidation of a redox couple lying close to the top of the O2-:2p6 valence band, and (3)the hydrogen-evolution reaction occurs at the surface OH2 species bonded to cations with a surface redox couple lying close to the H+H level in solution.

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Surface Protonation and Electrochemical Activity of Oxides in Aqueous Solution

Abstract

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