Tuning the oxygen vacancy and acidity of V-Ag-Ce/TiO2 catalyst for selective gas-phase oxidation of toluene to benzaldehyde

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2023-09-05 DOI:10.1016/j.apcata.2023.119381

Jiasheng Wang , Qingrong Wang , Mengdi Zhao , Ming Bao

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Abstract

Toluene gas-phase oxidation is a green, chlorine-free production process for benzaldehyde but its conversion efficiency is still unsatisfying due to the lack of highly efficient catalyst. Here the selective oxidation of toluene to benzaldehyde over V-Ag-Ce/TiO₂ under an air atmosphere was investigated. The catalyst was prepared by impregnation and characterized by scanning electron microscope (SEM), N₂ adsorption-desorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Electron paramagnetic resonance (EPR), H₂ temperature programmed reduction (H₂-TPR), O₂ temperature programmed desorption (O₂-TPD), and NH₃ temperature programmed desorption (NH₃-TPD). The amount of oxygen vacancy and acid of the catalyst can be tuned through adjusting the V:Ag:Ce ratio. Over the optimum catalyst (V:Ag:Ce = 4:2:1, molar ratio), 92% benzaldehyde selectivity with a 27% toluene conversion can be obtained at 550 °C. Medium amounts of oxygen vacancy (0.43) and acidity (0.10 mmol/g) are found to be conducive to the conversion of toluene to benzaldehyde. This study has important theoretical guiding significance for improving conversion efficiency from toluene to benzaldehyde by gas-phase aerobic oxidation.

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调节V-Ag-Ce/TiO2选择性气相氧化甲苯制苯甲醛催化剂的氧空位和酸度

甲苯气相氧化法是一种绿色、无氯的苯甲醛生产工艺，但由于缺乏高效的催化剂，其转化效率仍不理想。本文研究了在空气气氛下，在V-Ag-Ce/TiO2上甲苯选择性氧化制苯甲醛。采用浸渍法制备催化剂，并通过扫描电镜(SEM)、N2吸附-解吸、x射线衍射(XRD)、x射线光电子能谱(XPS)、电子顺磁共振(EPR)、H2程序升温还原(H2- tpr)、O2程序升温解吸(O2- tpd)、NH3程序升温解吸(NH3- tpd)等手段对催化剂进行表征。通过调节V:Ag:Ce的比例，可以调节催化剂的氧空位量和酸含量。在最佳催化剂(V:Ag:Ce = 4:2:1，摩尔比)条件下，在550℃下，苯甲醛选择性为92%，甲苯转化率为27%。中等氧空位(0.43)和酸度(0.10 mmol/g)有利于甲苯转化为苯甲醛。该研究对提高甲苯气相好氧制苯甲醛的转化效率具有重要的理论指导意义。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.