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Co/Fe 和 Co/Al 层状双金属氧化物臭氧催化剂用于苯胺的深度降解:制备、表征和动力学模型。

Co/Fe and Co/Al layered double oxides ozone catalyst for the deep degradation of aniline: Preparation, characterization and kinetic model.

机构信息

School of Environmental and Municipal Engineering, Qingdao University of Technology, Qingdao 266033, PR China; School of Environmental Science and Technology, Shandong University, Qingdao, 266237, PR China; Zhejiang Heze Envrionmental Tech Shares Co.,LTD, Huzhou, 313100, PR China.

School of Environmental and Municipal Engineering, Qingdao University of Technology, Qingdao 266033, PR China.

出版信息

Sci Total Environ. 2020 May 1;715:136982. doi: 10.1016/j.scitotenv.2020.136982. Epub 2020 Jan 28.

Abstract

In this work, Co/Fe and Co/Al layered double oxides (Co/Fe-LDO and Co/Al- LDO)ozone catalysts were obtained from Co/Fe and Co/Al layered double hydroxides intermediates (Co/Fe-LDH and Co/Al-LDH). Firstly, the optimal preparation parameters of the two intermediates were determined, then the morphology and mineralogy microstructure of the derived Co/Fe-LDO and Co/Al- LDO ozone catalysts were systematically studied. Finally, the reaction kinetics of the two ozone catalysts for the deep degradation of aniline wastewater in catalysts/ozone systems were established. The results showed that the optimal preparation conditions were set as pH 12, temperature 60 °C, cobalt‑iron ratio 3:1 for Co/Fe-LDH intermediate, and pH 12, temperature 70 °C, cobalt‑aluminum ratio 3:1 for Co/Al-LDH intermediate. During calcination treatment, the dehydration and recrystallization effect impelled LDH intermediate to form LDO catalyst. The derived ozone catalysts Co/Fe-LDO and Co/Al-LDO possess layered structure, and Co species was mainly based on CoO as the main mineral phase of the two ozone catalysts. The addition of catalyst can realize the deep ozonation catalysis of aniline wastewater. The kinetic models established on the aniline oxidized by ozone or catalyst/ozone systems were both fitted the first-order reactions, and the reaction activation energy for COD and TOC degradation were significantly reduced in catalyst/ozone system.

摘要

在这项工作中,从 Co/Fe 和 Co/Al 层状双氢氧化物中间体(Co/Fe-LDH 和 Co/Al-LDH)获得了 Co/Fe 和 Co/Al 层状双氧化物(Co/Fe-LDO 和 Co/Al-LDO)臭氧催化剂。首先,确定了两种中间体的最佳制备参数,然后系统研究了衍生的 Co/Fe-LDO 和 Co/Al-LDO 臭氧催化剂的形貌和矿物微观结构。最后,在催化剂/臭氧体系中建立了两种臭氧催化剂深度降解苯胺废水的反应动力学。结果表明,Co/Fe-LDH 中间体的最佳制备条件为 pH 12、温度 60°C、钴铁比 3:1,Co/Al-LDH 中间体的最佳制备条件为 pH 12、温度 70°C、钴铝比 3:1。在煅烧处理过程中,脱水和重结晶作用促使 LDH 中间体形成 LDO 催化剂。衍生的臭氧催化剂 Co/Fe-LDO 和 Co/Al-LDO 具有层状结构,Co 物种主要以 CoO 为两种臭氧催化剂的主要矿物相。催化剂的添加可以实现苯胺废水的深度臭氧催化。在臭氧或催化剂/臭氧体系中氧化苯胺建立的动力学模型均符合一级反应,并且在催化剂/臭氧体系中 COD 和 TOC 降解的反应活化能显著降低。

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