| Summary: | The influence of Yb<sup>3+</sup> cations substitution for Pr<sup>3+</sup> on the structure and catalytic activity of (Pr<sub>1−<i>x</i></sub>Yb<sub><i>x</i></sub>)<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> powders synthesized via coprecipitation followed by calcination is studied using a combination of long- (s-XRD), medium- (Raman, FT-IR, and SEM-EDS) and short-range (XAFS) sensitive methods, as well as adsorption and catalytic techniques. It is established that chemical composition and calcination temperature are the two major factors that govern the phase composition, crystallographic, and local-structure parameters of these polycrystalline materials. The crystallographic and local-structure parameters of (Pr<sub>1−<i>x</i></sub>Yb<sub><i>x</i></sub>)<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> samples prepared at 1400 °C/3 h demonstrate a tight correlation with their catalytic activity towards propane cracking. The progressive replacement of Pr<sup>3+</sup> with Yb<sup>3+</sup> cations gives rise to an increase in the catalytic activity. A mechanism of the catalytic cracking of propane is proposed, which considers the geometrical match between the metal–oxygen (Pr–O, Yb–O, and Zr–O) bond lengths within the active sites and the size of adsorbed propane molecule to be the decisive factor governing the reaction route.
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