棓酸增强碳基材料活化过一硫酸盐降解对硝基苯酚  

Gallic acid reinforced carbon-based materials for peroxymonosulfate activation to p-nitrophenol degradation

作　　者：冉越 张英 何丕文[1] 龙杰 殷涛[1] 彭峰[1] RAN Yue;ZHANG Ying;HE Piwen;LONG Jie;YIN Tao;PENG Feng(School of Urban Construction,Yangtze University,Jingzhou 434023,Hubei,China;Longquan Township Urban and Rural Construction Office,Yichang 443112,Hubei,China)

机构地区：[1]长江大学城市建设学院,湖北荆州434023 [2]龙泉镇城乡建设办公室,湖北宜昌443112

出　　处：《精细化工》2024年第12期2744-2753,共10页Fine Chemicals

基　　金：湖北省自然科学基金项目(2017CFB327)。

摘　　要：以含油污泥(OS)为原料,采用一步热解法制备了含油污泥碳基材料(OSC),将其作为过一硫酸盐(PMS,过硫酸氢钾)的非均相活化剂用于降解对硝基苯酚(PNP)。通过XRD、SEM、EDS、XPS表征了样品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p H、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Fe^(3+)/Fe^(2+)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体系中表现出最佳的活化性能,在OSC-800料液比(g∶L)2∶1、溶液初始p H=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·SO_(4)^(-)、·OH、·O_(2)^(–)和单线态氧4种活性物种。Oily sludge carbon-based materials (OSC) were prepared from pyrolysis of oily sludge (OS),used as heterogeneous activator for permonosulfate (PMS,potassium peroxymonosulfate) to degrade p-nitrophenol (PNP),and characterized by XRD,SEM,EDS and XPS for analysis on the microscopic morphology and elemental valence.The effects of different reaction systems,pyrolytic temperature of carbon-based material,gallic acid (GA) concentration,PMS concentration,initial solution p H,reaction temperature,PNP mass concentration,co-existing anion type and xanulinic acid (FA) mass concentration on the degradation of PNP by OSC activated PMS were evaluated.The results demonstrated that the surface hydroxyl groups on OSC-800 and the valence cycle between Fe^(3+) and Fe^(2+)were involved in the activation of PMS,and GA introduction greatly accelerated PNP degradation,with the OSC-800 prepared at 800℃showing the best activation performance in the OSC-800/PMS/GA system.Under the conditions of OSC-800 solid-liquid ratio (g∶L) 2∶1,initial solution p H 6.7,PMS concentration 1.4 mmol/L,GA concentration 0.25 mmol/L,PNP mass concentration 20 mg/L and reaction temperature 25℃,the PNP degradation rate reached 88.14%within 100 min.The PNP degradation rate constant (0.0191 min^(-1)),COD removal rate (76.01%) and PMS utilization rate (93.44%) were increased by 194%,65% and 190%compared with those of OSC-800/PMS system.OSC-800/PMS/GA system produced·SO_(4)^(-),·OH,·O_(2)^(-) and singlet oxygen in the reaction.

关 键 词：含油污泥 过一硫酸盐 棓酸 对硝基苯酚 降解机制 水处理技术 

分 类 号：TQ426[化学工程] X703[环境科学与工程—环境工程]