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Abstract:
Efficient development of catalytic materials requires knowledge of the decisive parameters defining the catalytic properties. In multicomponent metallic catalysts, these are categorized as electronic and geometric effects, yet they are strongly interrelated. A systematic disentanglement can be achieved by fixing one parameter while altering the other, which becomes possible through the substitution in isostructural intermetallic compounds. This approach enables the evaluation of electronic or geometric contributions both individually and combined. Herein, this is achieved by substitution of indium (three valence electrons) with tin (four valence electrons) in the series In(1-x)SnxPd(2), which allows for a systematic variation of the total number of electrons per unit cell with only a minor variation of the unit cell parameters and thus the evaluation of the electronic effect. Geometric effects were evaluated by substitution of indium with gallium in the Ga(1-x)InxPd(2) series, which allows for a systematic variation of the interatomic distances while maintaining the same number of valence electrons per unit cell and close atomic coordinates. By substituting gallium with tin in the Ga(1-x)SnxPd(2) series, both effects are combined and addressed simultaneously. The activity enhancement of the methanol oxidation reaction on the Ga(1-x)SnxPd(2) series is attributed to the synergy of the combined effects.
