Co NCP非均相催化过硫酸盐降解N,N二甲基甲酰胺的研究  

Degradation of N,N dimethylformamide by persulfate catalyzed by Co-NCP

作　　者：何争光[1] 席高阳 邢雨 陈树勋 张旭航 HE Zheng-guang;XI Gao-yang;XING Yu;CHEN Shu-xun;ZHANG Xu-hang(School of Ecology and Environment,Zhengzhou University,Zhengzhou 450001,China;School of Water Conservancy,Zhengzhou University,Zhengzhou 450001,China)

机构地区：[1]郑州大学生态与环境学院,郑州450001 [2]郑州大学水利科学与工程学院,郑州450001

出　　处：《安全与环境学报》2023年第1期261-267,共7页Journal of Safety and Environment

基　　金：国家科技重大专项(2017ZX07602-001-002)。

摘　　要：采用煅烧-浸渍法制备了钴改性天然黄铜矿(Co-NCP)高效催化剂,并采用Co-NCP活化过一硫酸盐(PMS)对N,N-二甲基甲酰胺(DMF)进行氧化降解。采用扫描电子显微镜(SEM)、X射线衍射仪(XRD)、能量-色散光谱(EDS)对Co-NCP反应前后的理化性质进行表征。结果表明煅烧后的天然黄铜矿的粗糙度变大,颗粒排布也更加紧密,可以提高浸渍法制备催化剂的性能。系统地研究了Co-NCP催化剂的投加量和PMS的投加量、初始pH值对反应体系的影响,确定了该反应的最优参数。结果表明,在中性条件下,Co-NCP投加量为4.0 g/L、PMS为4.0 g/L时,质量浓度为120 mg/L的DMF水溶液可以在40 min内达到91.61%的降解率。根据动力学方程对Co-NCP活化PMS降解DMF反应进行拟合,结果表明该反应符合准一级反应动力学。不同体系反应的动力学速率常数显示Co-NCP/PMS体系反应速率远大于其他反应体系,说明Co-NCP催化剂对PMS有高效的活化作用。通过自由基淬灭试验以及电子顺磁共振(EPR)分析结果表明体系中的活性物种有OH·、SO_(4)^(-)·和^(1)O_(2),其中SO_(4)^(-)·、OH·是主要的活性物种,采用电感耦合等离子体质谱(ICP-MS)分析得出反应过程中有少量的金属溶出,但溶出量不大。该研究确定了Co-NCP体系降解DMF的最佳反应条件并阐明了反应机理,对含DMF废水的处理具有一定的指导意义。In this work,we prepared an efficient catalyst for cobalt-modified natural chalcopyrite(Co-NCP)by a calcination-impregnation method and activated peroxymonosulfate(PMS)by Co-NCP for N,N dimethylformamide(DMF)for oxidative degradation.The physicochemical properties of Co-NCP before and after the reaction were characterized by scanning electron microscopy(SEM),X-ray diffraction(XRD),and energy-dispersive spectroscopy(EDS).It can be inferred that the roughness of calcined natural chalcopyrite becomes more extensive and the grain arrangement is closer,which can improve the efficiency of catalyst preparation by the impregnation method.The effects of Co-NCP catalyst dosage,PMS dosage,and initial pH value on the reaction system were systematically studied,and the optimal parameters of the reaction were determined.The results show that under neutral conditions,when the Co-NCP dosage is 4.0 g/L,and PMS is 4.0 g/L,DMF solution with a concentration of 120 mg/L can achieve a 91.61%degradation rate within 40min.According to the kinetic equation,the reaction of Co-NCP activation PMS degradation DMF was fitted.The results show that the reaction conforms to the quasifirst-order kinetics.According to the reaction kinetic rate constants of different reaction systems,it can be concluded that the Co-NCP/PMS reaction system is much larger than other reaction systems,indicating that the Co-NCP catalyst has an efficient activation effect on PMS.The results of the free radical quenching experiment and electron paramagnetic resonance(EPR)analysis showed that the active species in the system were OH·,SO_(4)^(-)·,and ^(1)O_(2),among which OH·and SO_(4)^(-)·were the main active species.Inductively coupled plasma mass spectrometry(ICP-MS)analysis showed that a small amount of metal was leaching during the reaction process,but the leaching amount was not significant.In this study,the optimal reaction conditions for degradation of DMF in Co-NCP system were determined,and the reaction mechanism was elucidated,which is of great guiding signi

关 键 词：环境工程学 N N-二甲基甲酰胺 Co-NCP 过一硫酸盐 氧化降解 

分 类 号：X52[环境科学与工程—环境工程]