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Effectiveness of toluene mineralisation by gas phase oxidation over Co(II)/SiO2 catalyst with ozone.
Environmental Technology ( IF 2.2 ) Pub Date : 2020-05-18
Piotr Machniewski, Andrzej Biń, Katarzyna Kłosek

The results of experimental study on effectiveness of gas phase total oxidation of toluene towards carbon dioxide and water with the aid of ozone over Co(II)/ SiO2 catalyst are presented in this work. The main objective of the work was to determine ozone demand necessary for total mineralisation of toluene at the temperature range of 40 -100 °C chosen to minimise catalyst poisoning by water.Completemineralisation of toluene was possible if sufficient ozone/toluene ratio was maintained in the gas supplied to the reactor. For ozone/toluene molar ratios less than 20 the extent of toluene mineralization increased with temperature up to a plateau starting at approximately 60°C,which was caused by ozone shortage. Stoichiometry of the total oxidation of toluene with ozone indicates that only one oxygen atom in theozone molecule is used for the oxidation of toluene, to achieve complete mineralisation. Experimentally determined ozone/toluene ratio (20-25) necessary for the total oxidation of toluene was larger than the theoretical one mostly due to ozone losses resulting from its “unproductive” decomposition. At the range of lower values of mineralisation ratethe toluene oxidation proceeds according toa more efficient mechanism, indicating less ozone demand being between 6 and 18 moles of ozone per mole of toluene. A possible mechanism of toluene oxidation was suggested. The mechanism involves the formation of OH radicals, which may explain the effectiveness of Co(II)/ SiO2 catalyst in combination with ozone for the oxidation of toluene andother aromatic VOCsin a low-temperature process.



中文翻译:

用臭氧在Co(II)/ SiO2催化剂上进行气相氧化制甲苯的有效性。

Co(II)/ SiO 2上臭氧辅助甲苯气相​​全氧化为二氧化碳和水的实验研究结果催化剂在这项工作中提出。这项工作的主要目的是确定在40 -100°C的温度范围内甲苯全部矿化所必需的臭氧需求,选择该温度范围以最大程度地降低催化剂对水的中毒。供入反应器的气体。对于小于20的臭氧/甲苯摩尔比,甲苯的矿化程度随温度升高而升高,直到大约60°C达到平稳状态,这是由臭氧短缺引起的。甲苯与臭氧的总氧化的化学计量表明,臭氧分子中只有一个氧原子可用于甲苯的氧化,以实现完全矿化。实验确定的甲苯总氧化所需的臭氧/甲苯比(20-25)大于理论值,这主要是由于其“非生产性”分解所导致的臭氧损失。在较低的矿化速率值范围内,甲苯氧化会根据更有效的机理进行,这表明较少的臭氧需求量为每摩尔甲苯6至18摩尔臭氧。提出了甲苯氧化的可能机理。该机制涉及 提出了甲苯氧化的可能机理。该机制涉及 提出了甲苯氧化的可能机理。该机制涉及 OH自由基,可以解释Co(II)/ SiO 2催化剂与臭氧结合在低温过程中氧化甲苯和其他芳族VOC的有效性。

更新日期:2020-05-18
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