催化作用
氧化还原
化学
平衡(能力)
无机化学
有机化学
医学
物理疗法
作者
Xiaohan Guo,Siyuan Sun,Meixingzi Gao,Qiguang Dai,Wangcheng Zhan,Li Wang,Yun Guo,Yun Guo,Ai‐Yong Wang,Yang‐Long Guo,Yang‐Long Guo
出处
期刊:Rare Metals
[Springer Science+Business Media]
日期:2024-07-15
卷期号:43 (12): 6473-6485
被引量:12
标识
DOI:10.1007/s12598-024-02889-1
摘要
Abstract Due to the presence of nitrogen, nitrogen‐containing volatile organic compounds (NVOCs) are more difficult to remove than conventional volatile organic compounds (VOCs). Both catalytic activity and N 2 selectivity should be considered in the design of suitable catalysts. A series of Ag/Ce–Zr solid solution (Ag/CZ) catalysts were prepared and applied to the catalytic oxidation of N,N‐dimethylformamide (DMF). Redox ability and acidity were regulated by modifying the Zr content. The introduction of Zr promoted the formation of active oxygen species until the molar ratio of Zr reached 0.5, after which the formation decreased. Moreover, adding Zr increased the number of weak and medium acidic sites, which significantly improved DMF adsorption. The improved DMF adsorption hindered the combination of nitrogen and active oxygen, thus reducing the generation of NO x effectively. Therefore, the Ag/CZ (5:5) catalyst, with suitable redox ability and acidity, exhibited the highest activity ( T 90 = 176 °C), the lowest elimination temperature of organic compounds ( T = 255 °C), satisfactory N 2 yield (95%–75% in the range of 240–400 °C), and outstanding stability under both common and humid conditions (at least 50 h). The reaction mechanism was investigated based on the in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results. During the catalytic oxidation of DMF, the surface lattice oxygen directly participated in the dehydrogenation and dissociation of the C(O)–N bonds. The generated dimethylamine (DMA) was then oxidized by active oxygen species to form the final product.
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