The role of WOx and dopants (ZrO2 and SiO2) on CeO2-based nanostructure catalysts in the selective oxidation of benzyl alcohol to benzaldehyde under ambient conditions

WOx 和掺杂剂(ZrO2 和 SiO2)在环境条件下对 CeO2 基纳米结构催化剂在苯甲醇选择性氧化为苯甲醛中的作用

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作者:Ganeshbabu Bathula, Surjyakanta Rana, Siddaramagoud Bandalla, Vijaykumar Dosarapu, Satyanarayana Mavurapu, Aswathi Rajeevan V V, Bhaskar Sharma, Sreekantha B Jonnalagadda, Mallesham Baithy, Chandra Shekar Vasam

Abstract

Herein, the efficacy of WOx-promoted CeO2-SiO2 and CeO2-ZrO2 mixed oxide catalysts in the solvent-free selective oxidation of benzyl alcohol to benzaldehyde using molecular oxygen as an oxidant is reported. We evaluated the effects of the oxidant and catalyst concentration, reaction duration, and temperature on the reaction with an aim to optimize the reaction conditions. The as-prepared CeO2, CeO2-ZrO2, CeO2-SiO2, WOx/CeO2, WOx/CeO2-ZrO2, and WOx/CeO2-SiO2 catalysts were characterized by X-ray diffraction (XRD), N2 adsorption-desorption, Raman spectroscopy, temperature-programmed desorption of ammonia (TPD-NH3), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). These characterisation results indicated that the WOx/CeO2-SiO2 catalyst possessed improved physicochemical (i.e., structural, textural, and acidic) properties owing to the strong interactivity between WOx and CeO2-SiO2. A higher number of Ce3+ ions (Iu'''/ITotal) were created with the WOx/CeO2-SiO2 catalyst than those with the other catalysts in this work, indicating the generation of a high number of oxygen vacancies. The WOx/CeO2-SiO2 catalyst exhibited a high conversion of benzyl alcohol (>99%) and a high selectivity (100%) toward benzaldehyde compared to the other promoted catalysts (i.e., WOx/CeO2 and WOx/CeO2-ZrO2), which is attributed to the smaller particle size of the WOx and CeO2 and their high specific surface area, more significant number of acidic sites, and superior number of oxygen vacancies. The WOx/CeO2-SiO2 catalyst could be quickly recovered and utilized at least five times without suffering any appreciable activity loss.

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