棓酸增强碳基材料活化过一硫酸盐降解对硝基苯酚
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1.长江大学城市建设学院;2.龙泉镇城乡建设办公室

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湖北省自然科学基金(2017CFB327)


Gallic acid reinforced carbon-based materials activate peroxymonosulfate to degrade p-nitrophenol
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1.School of Urban Construction,Yangtze University;2.Longquan Township Urban and Rural Construction Office

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Natural Science Foundation of Hubei Province [No. 2017CFB327]

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    摘要:

    以含油污泥(OS)为原料,采用一步热解法制备含油污泥碳基材料OSC,将其作为过一硫酸盐(PMS)的非均相活化剂用于降解对硝基苯酚(PNP)。通过XRD、SEM、EDS、XPS表征了OSC的微观形貌结构和元素价态,考察了不同反应体系、热解碳基材料温度、棓酸(GA)浓度、PMS浓度、溶液初始pH、反应温度、PNP质量浓度、共存阴离子类型、黄腐酸(FA)质量浓度对OSC活化PMS降解PNP的影响,探讨了PNP降解机制。结果表明,OSC上的表面羰基及Fe3+/Fe2+之间的价态循环参与了PMS的活化,GA的引入明显增强了PNP的降解。热解碳基材料温度800 ℃制备的OSC-800在OSC-800/PMS/GA催化体系中表现出最佳的活化性能,当OSC-800料液比(g∶L)2∶1,溶液初始pH=6.7,PMS浓度1.4 mmol/L,GA浓度0.25 mmol/L,PNP质量浓度20 mg/L,反应温度25 ℃的条件下,100 min内PNP降解率为88.14%,其降解过程符合准一级动力学模型,其对PNP的降解速率常数(0.0191 min?1)比OSC-800/PMS体系提升了194%,COD去除率(76.01%)提高了65%,PMS的利用率(93.44%)提高了190%。OSC-800/PMS/GA体系在反应中产生了·SO4?、·OH、·O2–和1O2这4种活性物种。

    Abstract:

    Oily sludge carbon-based materials (OSC-X, X represents the calcination temperature, 500,600,700,800 and 900 °C, respectively) were prepared by pyrolysis method, and SEM, EDS, XRD, and XPS were used to analyze the microscopic morphology and elemental valence of the materials. On the degradation of p-nitrophenol (PNP) by OSC-800/PMS/GA, the effects of various systems, the temperature at which the carbon-based materials were pyrolyzed, the mass concentrations of gallic acid (GA) and peroxymonosulfate (PMS), the initial pH of the solution, the reaction temperature, and the concentration of pollutants were examined,the mechanism of PNP degradation by OSC-800/PMS/GA was explored. The findings demonstrated that the valence cycle between Fe3+ and Fe2+ and the surface hydroxyl groups on OSC-800 were involved in the activation of PMS and that adding GA greatly accelerated OSC-800 of catalytic degradation of PNP. The degradation rate of PNP by this system (OSC-800/PMS/GA) at 100 min was 88.14%, and the degradation process was consistent with the quasi-primary kinetic model. These conditions included an OSC-800 mass concentration of 2 g/L, a solution initial pH of 6.7, PMS molar concentration of 1.4 mmol/L, GA molar concentration of 0.25 mmol/L, PNP mass concentration of 20 mg/L, and a reaction temperature of 25 °C. There was a 2.42-fold increase in the degradation rate constant of PNP compared to the OSC-800/PMS system, a 1.65-fold increase in the COD elimination rate, and a 2.94-fold increase in the PMS utilization rate. Four kinds of reactive oxygen species (ROS), SO4??, ?OH, ?O2? and 1O2 were produced during the reaction.

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冉越,张英,何丕文,龙杰,殷涛.棓酸增强碳基材料活化过一硫酸盐降解对硝基苯酚[J].精细化工,2024,41(12):

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  • 收稿日期:2024-07-19
  • 最后修改日期:2024-08-28
  • 录用日期:2024-08-22
  • 在线发布日期: 2024-12-10
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