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One-step synthesis of transition metal modified UiO-66-Ce metal-organic framework: Catalytic oxidation of toluene and investigation of the mechanism
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2022-09-26 , DOI: 10.1016/j.micromeso.2022.112214
Xueyan Hou , Ye Bian , Linjun Yang

As a kind of VOCs, the direct catalytic oxidation of toluene to CO2 and H2O is a great challenge. A high-performance catalyst plays a crucial role in catalytic oxidation. Herein, UiO-66-Ce and a series of transition metals-doped UiO-66-CeM (M = Cu, Co, Mn, Fe, Zr) through a rapid and facile one-step synthesis method are prepared to investigate the catalytic oxidation of toluene. Experiments disclose that the UiO-66-CeCu exhibits extremely high catalytic capacity. A range of characterizations reveals that the oxygen vacancies formed between Ce and the doped metal. Better redox performance play a key role in the oxidation of toluene (Ce4++Mn+→Ce3++M(n+1)+). Most importantly, the analysis of the catalytic oxidation mechanism in situ DRIFTS in different conditions. Concluded that toluene oxidation is the coexistence of MvK mechanism and L-H mechanism. Furthermore, the oxygen vacancies increase the mobility of gaseous oxygen on the surface, which is essential in improving catalytic activity. Finally, the degradation pathway of toluene in UiO-66-CeM was concluded as follows: toluene → benzyl alcohol → benzoic acid → acid anhydride …...CO2 and H2O.



中文翻译:

过渡金属改性UiO-66-Ce金属-有机骨架的一步合成:甲苯的催化氧化及机理研究

作为VOCs的一种,甲苯直接催化氧化成CO 2和H 2 O是一个很大的挑战。高性能催化剂在催化氧化中起着至关重要的作用。本文通过快速简便的一步合成方法制备了 UiO-66-Ce 和一系列过渡金属掺杂的 UiO-66-CeM (M = Cu, Co, Mn, Fe, Zr),用于研究催化氧化甲苯。实验表明,UiO-66-CeCu 表现出极高的催化能力。一系列表征表明,在 Ce 和掺杂金属之间形成了氧空位。较好的氧化还原性能在甲苯的氧化中起关键作用(Ce 4+ +M n+ →Ce 3+ +M (n+1)+)。最重要的是分析了不同条件下原位DRIFTS的催化氧化机理。得出甲苯氧化是MvK机制和LH机制并存的结果。此外,氧空位增加了气态氧在表面上的流动性,这对于提高催化活性至关重要。最后得出甲苯在UiO-66-CeM中的降解途径为:甲苯→苯甲醇→苯甲酸→酸酐……CO 2和H 2 O。

更新日期:2022-09-26
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