湿式催化氧化法处理高浓度高盐毒死蜱废水
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重庆市教委项目(KJQN201901512);重庆市科技局自然科学基金项目(CSTC2020JCYJ-MSXMX0489)


High-salt chlorpyrifos wastewater treated by Catalystic Wet Air Oxidation
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    摘要:

    以γ-Al2O3为载体,通过超声浸渍法制备Mn-Ce/γ-Al2O3,并以其为催化剂采用湿式催化氧化法处理高浓度高盐毒死蜱废水。通过FTIR、XRD、SEM对催化剂结构进行表征。通过单因素实验探讨了反应温度、pH、催化剂用量、氧化剂用量对COD去除率的影响。采用均匀设计法对湿式催化氧化实验条件进行优化,在进水COD质量浓度为13550 mg/L时,最优处理条件为反应温度230 oC,反应时间2 h,进水pH=7,质量分数30%过氧化氢5.5 mL,Mn-Ce/γ-Al2O3用量0.4 g,在该条件下,COD去除率达到90.63%;各因素影响实验结果的主次顺序为反应温度>催化剂用量>氧化剂用量>pH>反应时间。采用DFT方法计算毒死蜱分子的量子化学参数,结合自由基捕获实验和紫外光谱结果初步探讨了湿式催化氧化降解毒死蜱的可能机理。结果表明,γ-Al2O3上负载了MnO2、CeO2活性组分,Mn-Ce/γ-Al2O3能较好地促进H2O2产生•OH;动力学实验表明,湿式催化氧化对废水COD的降解过程符合准二级动力学方程。

    Abstract:

    Using γ-Al2O3 as carrier, Mn-Ce/γ-Al2O3 was prepared by ultrasonic impregnation method, and it was used as catalyst to treat high-concentration and high-salt chlorpyrifos wastewater by catalytic wet air oxidation. The catalytic materials were characterized by FTIR, XRD, SEM. By single factor experiment, this paper discusses the reaction temperature, pH, catalyst dosage, the dosage of oxidant on the influence law of COD removal. The uniform design method was used to optimize the experimental conditions of catalytic wet air oxidation, when the influent COD concentration is 13550 mg/L, the optimal conditions of wet catalytic oxidation are as follows: reaction temperature is 230 oC, reaction time is 2 h, influent pH is 7, dosage of 30% hydrogen peroxide is 5.5 mL, dosage of Mn-Ce/γ-Al2O3 catalyst is 0.4 g, under this condition, COD removal rate reaches 90.63%; the primary and secondary order of various factors affecting the experimental results is reaction temperature > amount of catalyst > amount of oxidant > time. The density functional theory method is used to calculate the quantum chemical parameters of chlorpyrifos molecule, combined with free radical capture experiment and the results of the UV spectrum, the possible mechanism of catalytic wet air oxidation degradation of chlorpyrifos was preliminarily discussed. the results show that, MnO2 and CeO2 active components are loaded on γ-Al2O3, Mn-Ce/γ-Al2O3 can better promote H2O2 to produce •OH, and The kinetic experiments show that the degradation process of COD by catalystic wet air oxidation is in line with the quasi-second-order kinetic equation.

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胡诗越,原金海,唐倩.湿式催化氧化法处理高浓度高盐毒死蜱废水[J].精细化工,2022,39(4):

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  • 收稿日期:2021-10-26
  • 最后修改日期:2021-12-27
  • 录用日期:2021-12-28
  • 在线发布日期: 2022-01-29
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