Synergistically Enhanced Oxygen Evolution Reaction Catalysis for Multielement Transition-Metal Oxides
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Abstract
Transition metal oxides have been extensively investigated as novel catalysts for oxygen evolution reaction (OER). Partial elemental substitutions are effective ways to increase catalytic performance and such electronic interactions between multiple elements are known as synergistic effects. However, serious issues such as random atomic arrangement and ambiguous roles of constituent elements humper theoretical investigations for rational materials design. Herein, we describe systematic study on OER activity of AA′3B4O12-type quadruple perovskite oxides, in which multiple transition metal ions are located at distinct crystallographic sites. Electrochemical measurements demonstrate that OER catalytic activities of quadruple perovskite oxide series, CaCu3B4O12 (B = Ti, V, Cr, Mn, Fe, and Co), are all superior to those of simple perovskite counterparts CaBO3. The order of activity of B-site transition metal ions for CaBO3 (Fe4+ > Co4+ ≫ Ti4+, V4+, Cr4+, Mn4+) is retained in CaCu3B4O12, indicating that B-site ions play a primary role whereas A′-site Cu ions secondarily contribute to OER activity for CaCu3B4O12. Charge-transfer energies, energy differences between oxygen 2p band center and unoccupied 3d band center of B-site transition metal obtained from first-principles electronic-state calculations, illustrate that OER overpotentials of quadruple perovskite oxides are lower than simple perovskite oxides by ∼150 mV. These findings propose a simple avenue to realize enhanced OER activity for multiple transition-metal ions.
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