CuCe/ZSM-5复合材料的制备及降解有机废水研究  

Study on Preparation of CuCe/ZSM-5 Composite Material and Degradation of Organic Wastewater

作　　者：许洪祝 李长波[1] 赵国峥[1] 王硕[1] 梁慧 付玉婷 孙子凯 杨佳潼 李东彧 张岱航 XU Hongzhu;LI Changbo;ZHAO Guozheng;WANG Shuo;LIANG Hui;FU Yuting;SUN Zikai;YANG Jiatong;LI Dongyu;ZHANG Daihang(School of Environmental and Safety Engineering,Liaoning Petrochemical University,Fushun 113001,Liaoning,China)

机构地区：[1]辽宁石油化工大学环境与安全工程学院,辽宁抚顺113001

出　　处：《材料导报》2022年第24期219-225,共7页Materials Reports

基　　金：国家水体污染控制与治理科技重大专项(2012ZX07202-002);辽宁省教育厅重点攻关项目(L2020003);辽宁省教育厅项目(L2020020)。

摘　　要：使用微波辅助合成法制备CuCe/ZSM-5催化剂,通过改变反应温度、初始pH和催化剂添加量,研究CuCe/ZSM-5催化剂在含酚废水和工业污水中化学需氧量(COD)去除率的变化情况。采用XRD、XPS、SEM、TEM等手段对催化剂进行表征,结果显示,CuCe固溶体的形成可以加速Cu^(+)/Cu^(2+)和Ce^(4+)/Ce^(3+)离子对之间的电荷转换,促进H_(2)O_(2)分子被活化形成强氧化性物种。CuCe/ZSM-5显示出高活性和稳定性,其可以在75℃下180 min内达到90%的COD去除率,且连续使用五次仍保持稳定。含酚废水和工业污水的催化湿式过氧化氢氧化法(CWPO)反应符合一级动力学方程的动态模拟曲线,工业污水中污染物成分复杂且比含酚废水更难降解。利用GC-MS全面分析降解过程中产生的中间产物发现,苯酚经过脱氢、开环和氧化等多个步骤生成乙酸等中间产物,最终矿化生成CO_(2)和H_(2)O等小分子物质。CuCe/ZSM-5 catalysts were prepared by microwave-assisted synthesis,and the changes of chemical oxygen demand(COD)removal rate of CuCe/ZSM-5 catalysts in phenol-containing wastewater and industrial wastewater were studied by changing the reaction temperature,initial pH and catalyst addition amount.The catalyst was characterized by XRD,XPS,SEM,TEM and other methods,and the results show that the formation of CuCe solid solution can accelerate the charge conversion between Cu^(+)/Cu^(2+)and Ce^(4+)/Ce^(3+)ion pairs,and promote the activation of H_(2)O_(2) molecules to form strong oxidizing species.CuCe/ZSM-5 shows high activity and stability,and it can achieve a COD removal rate of 90%within 180 min at 75℃and remain stable after five consecutive uses.The catalytic wet hydrogen peroxide oxidation(CWPO)reaction of phenol-containing wastewater and industrial wastewater conforms to the dynamic simulation curve of the first-order kinetic equation,and the complex pollutant composition in industrial wastewater is more difficult to degrade than that of phenol-containing wastewater.GC-MS was used to comprehensively analyze the intermediate products generated during the degradation process,and it was found that phenol was dehydrogenated,ring-opening and oxidized to generate intermediates such as acetic acid,and finally mineralized to generate small molecules such as CO_(2) and H_(2)O.

关 键 词：催化湿式过氧化氢氧化 连续流 有机废水 动力学研究 机理分析 

分 类 号：O643.36[理学—物理化学]