Catalytic performance and mechanism of toluene oxidation in high humidity over the mesoporous titania-ceria-supported Pt or Pd catalysts

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-04-07 DOI:10.1016/j.apcata.2025.120277

Fuping Xu , Jia Wang , Yutong Zhao , Hongxia Lin , Hongxia Chen , Yi Zhang , Xuefeng Wei , Hongxing Dai

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Abstract

The major challenges encountered in developing catalysts for volatile organic compound (VOCs) treatments by catalytic oxidation are related to the low-temperature oxidation performance and water resistance. To address these issues, we herein develop an in situ hard-templating method to prepare the Pt or Pd/mesoporous TiO₂-CeO₂ catalyst and apply it for the oxidation of toluene. It was found that the Pt/mesoporous TiO₂-CeO₂ catalyst exhibited outstanding catalytic performance and stability under the high humidity (15 vol% H₂O) condition. Various characterization results revealed that the Pt/meso-TiO₂-CeO₂ catalyst exhibited excellent catalytic activity: the temperatures at toluene conversions of 50 and 90 % were 195 and 214 °C at a space velocity of 30,000 mL g⁻¹ h⁻¹, with the TOF_Pt values and specific reaction rates at 160 and 180 °C being 70.34 × 10⁻³ and 153.13 × 10⁻³ s⁻¹, and 1.80 and 3.92 mmol g_Pt⁻¹ s⁻¹, respectively. Such excellent performance of Pt/meso-TiO₂-CeO₂ was related to its high surface area, abundant oxygen vacancies, high active oxygen species concentration, good low-temperature reducibility, and strong interaction between Pt or Pd and meso-TiO₂-CeO₂. The mechanism of toluene oxidation might take place via the following route: Toluene is first oxidized to benzyl alcohol and benzoquinone, then converted to benzaldehyde, benzoic acid, maleic anhydride, and these intermediates are finally oxidized to CO₂ and H₂O.

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介孔钛-铈负载Pt或Pd催化剂在高湿条件下对甲苯氧化的催化性能及机理

催化氧化处理挥发性有机化合物（VOCs）的催化剂开发面临的主要挑战与低温氧化性能和耐水性有关。为了解决这些问题，我们开发了一种原位硬模板方法来制备Pt或Pd/介孔TiO2-CeO2催化剂，并将其应用于甲苯的氧化。结果表明，Pt/介孔TiO2-CeO2催化剂在高湿（15 vol% H2O）条件下表现出优异的催化性能和稳定性。各种表征结果表明，Pt/介介tio2 - ceo2催化剂具有优异的催化活性：在空速为30,000 mL g−1 h−1时，甲苯转化率为50%和90%的温度分别为195和214 °C， 160和180 °C时的TOFPt值和比反应速率分别为70.34 × 10−3和153.13 × 10−3 s−1,1.80和3.92 mmol gPt−1 s−1。Pt/介观tio2 - ceo2的优异性能与其高表面积、丰富的氧空位、高活性氧浓度、良好的低温还原性以及Pt或Pd与介观tio2 - ceo2之间的强相互作用有关。甲苯的氧化机理可能通过以下途径发生：甲苯首先被氧化为苯甲醇和苯醌，然后转化为苯甲醛、苯甲酸、马来酸酐，这些中间体最后被氧化为CO2和H2O。

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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.