CuO-高岭石活化PMS降解诺氟沙星性能  

Catalytic performance of CuO-kaolinite composite for norfloxacin degradation by activating peroxymonosulfate

作　　者：姚绍武 钱伟民 王誉博 胡小龙[1] 张文彬 宋俊颖[2] 董雄波 YAO Shaowu;QIAN Weimin;WANG Yubo;HU Xiaolong;ZHANG Wenbin;SONG Junying;DONG Xiongbo(College of Energy and Mining Engineering,Shandong University of Science and Technology,Qingdao 266590,China;College of Safety and Environmental Engineering,Shandong University of Science and Technology,Qingdao 266590,China;Huzhou Xinkaiyuan Aggregate Co.,Ltd.,Huzhou 313002,China;Engineering Research Center of Nano-Geomaterials of Ministry of Education,China University of Geosciences(Wuhan),Wuhan 430074,China)

机构地区：[1]山东科技大学能源与矿业工程学院,山东青岛266590 [2]山东科技大学安全与环境工程学院,山东青岛266590 [3]湖州新开元碎石有限公司,浙江湖州313002 [4]中国地质大学(武汉)教育部纳米地质材料工程研究中心,湖北武汉430074

出　　处：《中国粉体技术》2024年第6期62-73,共12页China Powder Science and Technology

基　　金：国家自然科学基金项目,编号:52204289;山东省自然科学基金项目,编号:ZR2022QE236;青岛市自然科学基金项目,编号:23-2-1-107-zyyd-jch。

摘　　要：【目的】为解决纯过硫酸盐催化剂在制备过程中易团聚的问题,分析引入高岭石载体后催化剂的结构和催化性能的变化规律,实现对抗生素废水中有机污染物的高效降解。【方法】首先以高岭石为载体,采用水热煅烧法制备了CuO-高岭石复合材料;使用物相分析、X射线光电子谱、扫描电子显微镜和氮吸附仪等对材料的晶体结构、表面化学态、微观形貌、比表面积以及孔结构特征进行表征,考察不同CuO与高岭石质量比、催化剂用量和过一硫酸盐(peroxymonosulfate,PMS)用量对NOR降解效率的影响,进行实验条件优化,并系统分析CuO-高岭石复合材料催化PMS降解NOR的机制。【结果】CuO与高岭石质量比为40%时CuO-高岭石复合材料具有最优的催化性能,在催化剂质量浓度为1.5 g/L,PMS浓度为1.0 mmol/L,NOR初始质量浓度为10 mg/L,反应时间为60 min时,NOR的降解效率为76.21%;CuO-高岭石中Cu(Ⅰ)、Cu(Ⅱ)之间的价态循环参与PMS的活化,反应体系中主要的活性物种是单线态氧^(1)O_(2),而超氧自由基O_(2)^(·-)、硫酸根自由基SO_(4)^(·-)和羟基自由基·OH也参与NOR降解过程。【结论】CuO-高岭石复合材料中,CuO纳米片能够均匀地分散并沉积在高岭石载体表面,显著减少CuO纳米片的相互团聚,使得更多反应活性位点暴露,增强复合材料对PMS的活化能力和对NOR的降解能力。Objective Due to the overuse of pharmaceutical antibiotics,residues have been frequently detected in different environmental matrices,including surface water,sewage,and soils.The presence of antibiotics in environment can cause potential adverse effects on human and ecological system due to their acute and chronic toxicity and the development of antibiotic resistance.However,traditional wastewater purification technologies are ineffective in eliminating antibiotics.In recent years,the advanced oxidation process(AOP)based on sulfate radicals has been confirmed as the most suitable and efficient way to remove such pollutants from wastewater.The CuO-peroxymonosulfate(PMS)system,in particular,has gained considerable attention due to its strong oxidation ability.Nevertheless,the high surface energy of CuO often leads to aggregation during the synthesis process,reducing the amount of active sites and specific surface area.To address this problem,kaolinite was introduced as a support for CuO in this study,and changes in the structure and catalytic performance of the CuO-kaolinite catalyst were analyzed to achieve efficient degradation of organic pollutants in antibiotic wastewater.Methods In this paper,CuO-kaolinite composite was fabricated using a hydrothermal calcination method.Initially,1.0 g of sepiolite was mixed with 50 mL of distilled water and stirred for 0.5 h.Then,different amounts of Cu(NO_(3))_(2)·3H_(2)O were added to the solution and stirred for 10 min.Subsequently,an ammonia-water solution(v:v=1:1)was added drop-wise to adjust the pH value to 7.5~8 at room temperature.After stirring for 15 min,the mixture was transferred into a 100 mL Teflon-lined stainless-steel autoclave and heated at 150℃ for 5 h.The resulting products were washed,dried,ground,and then calcined in a muffle furnace at 250℃ for 3 h.Finally,after simple grinding,the CuO-kaolinite composite with different mass ratios of CuO and kaolinite was synthesized.The crystal structure,surface chemical state,microstructure,specific surface area,

关 键 词：CUO 高岭石 过硫酸盐催化剂 诺氟沙星 

分 类 号：TB44[一般工业技术] TD985[矿业工程—选矿]