4.6 Article

Influence of Synthesis Conditions on the Crystal, Local Atomic, Electronic Structure, and Catalytic Properties of (Pr1-xYbx)2Zr2O7 (0 ≤ x ≤ 1) Powders

期刊

CRYSTALS
卷 13, 期 9, 页码 -

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MDPI
DOI: 10.3390/cryst13091405

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praseodymium/ytterbium zirconates; crystal and local structures; catalytic cracking of propane; synchrotron XRD; X-ray absorption fine structure (XAFS); Raman spectroscopy; FT-IR spectroscopy

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This study investigates the influence of Yb3+ cations substitution for Pr3+ on the structure and catalytic activity of (Pr1-xYbx)(2)Zr2O7 powders. The results show that the chemical composition and calcination temperature play important roles in determining the phase composition, crystallographic, and local-structure parameters of these materials. The progressive replacement of Pr3+ with Yb3+ cations leads to an increase in catalytic activity.
The influence of Yb3+ cations substitution for Pr3+ on the structure and catalytic activity of (Pr1-xYbx)(2)Zr2O7 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 (Pr1-xYbx)(2)Zr2O7 samples prepared at 1400 degrees C/3 h demonstrate a tight correlation with their catalytic activity towards propane cracking. The progressive replacement of Pr3+ with Yb3+ 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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