Degradation of benzotriazole by a novel Fenton-like reaction with mesoporous Cu/MnO2: Combination of adsorption and catalysis oxidation
Degradation of benzotriazole by a novel Fenton-like reaction with mesoporous Cu/MnO2: Combination of adsorption and catalysis oxidation
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介孔 Cu/MnO2 的新型芬顿反应降解苯并三唑：吸附和催化氧化相结合
DOI：
10.1016/j.apcatb.2016.06.003
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发表时间：
2016-12
期刊：
影响因子：
--
通讯作者：
Chu Wei
中科院分区：
文献类型：
--
作者：
Zhang Yuting;Liu Cao;Xu Bingbing;Qi Fei;Chu Wei
以介孔MnO 2为载体制备了介孔Cu/MnO 2（MCM）催化剂，研究了新型类Fenton反应降解苯并三唑（BZA）的性能.采用N2吸附-脱附、X射线光电子能谱、紫外-可见漫反射光谱和程序升温还原（TPR）-H2等手段对催化剂进行了表征。通过中间体鉴定、XPS和TPR分析证实，MCM通过表面化学吸附和氧化还原反应发挥作用，随后通过表面Cu+和Mn 3+的类Fenton氧化作用，对溶液中的BZA提供了高的降解效率。傅里叶变换红外光谱（FT-IR）结果也证实了表面吸附和类Fenton反应。MCM在芬顿反应中表现出比纯MnO 2和CuO更高的吸附和催化活性。考察了MCM中Cu含量、催化剂用量、H2 O2用量、溶液pH等因素对反应的影响。BZA降解是高的去离子水（去除效率= 89%）和温和的污水处理厂的出水（去除效率= 56%），在60分钟的反应后，在初始pH值为7.13，这可以通过调整催化剂或H2 O2的剂量开发。提出了一种可能的反应机理。这涉及与铜的表面吸附和与Mn 3+的氧化还原反应，随后是铜-锰循环衍生的芬顿样反应。
Degradation of benzotriazole (BZA) as an emerging contaminant by a novel Fenton-like reaction was investigated using a catalyst prepared by incorporating Cu into mesoporous MnO2(mesoporous Cu/MnO2, MCM). Catalysts were synthesized with different Cu contents, and were characterized by N2adsorption–desorption, X-ray photoelectron spectroscopy, ultraviolet–visible (UV–vis) diffuse reflectance spectroscopy, and temperature-programmed reduction (TPR)-H2. The MCM functioned via surface chemisorption and redox reaction that was confirmed by intermediates identification, XPS and TPR analysis, followed by a Fenton-like oxidation derived by surface Cu+and Mn3+, to provide high degradation efficiency for BZA in solution. Fourier transform infrared (FT-IR) spectroscopy result also verified the surface adsorption and Fenton-like reaction. MCM exhibited much higher adsorption and catalytic activity in the Fenton reaction than pure MnO2or CuO. The effect of Cu content in MCM, catalyst dose, H2O2dose, and solution pH were investigated. BZA degradation was high in deionized water (removal efficiency = 89%) and moderate in wastewater treatment plant effluent (removal efficiency = 56%) after 60-min reaction at an initial pH of 7.13, which could be developed by adjusting the dose of catalyst or H2O2. A possible mechanism for the reaction is proposed. This involves surface adsorption with copper and a redox reaction with Mn3+, followed by a copper–manganese cycle-derived Fenton-like reaction.
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