湿式催化氧化降解焦化废水  

Catalytic wet oxidation degradation of coking wastewater

作　　者：马建超[1] 郭精茂 任凯文 张晓朋 鲍卫仁[2] 马清亮[2] MA Jianchao;GUO Jingmao;REN Kaiwen;ZHANG Xiaopeng;BAO Weiren;MA Qingliang(College of Mining Technology,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China;Key Laboratory of Coal Science and Technology,Taiyuan University of Technology,Ministry of Education and Shanxi Province,Taiyuan 030024,Shanxi,China)

机构地区：[1]太原理工大学矿业工程学院,山西太原030024 [2]太原理工大学煤科学与技术教育部和山西省重点实验室,山西太原030024

出　　处：《精细化工》2020年第10期2112-2119,共8页Fine Chemicals

基　　金：国家重点研发计划(2019YFC0408604-4);山西省重点研发计划(社会发展领域)(201903D321053);山西省自然科学基金(201801D121273,201901D111110);山西省留学回国人员科研项目(HGKY2019017);山西省优秀青年学术带头人项目。

摘　　要：以Cu(NO3)2·3H2O为原料,采用共沉淀法制备了CuMgLa/Al2O3催化剂,TEM和N2吸附-脱附结果表明,该催化剂具有介孔结构,主活性组分CuO的粒径约为25nm。以喹啉为降解目标污染物,考察了温度、催化剂质量浓度等对湿式催化氧化降解喹啉效果的影响。结果表明,当喹啉模拟废水质量浓度为1000mg/L,催化剂质量浓度为0.2 g/L,反应温度为240℃,O2分压为0.53 MPa,反应60 min时,喹啉去除率接近100.0%,化学需氧量(COD)去除率达到94.8%。通过UV光谱、LC-MS分析喹啉降解生成的中间体,结合叔丁醇淬灭实验,发现·OH氧化在湿式催化氧化降解喹啉体系中起主导作用,推测了喹啉可能的降解路径。在最优工艺条件下,COD质量浓度为7000mg/L的模拟焦化废水COD的去除率达94.6%;而COD质量浓度为4740.0 mg/L,NH3-N质量浓度为884.2 mg/L的实际焦化废水COD去除率为69.6%,NH3-N去除率为28.0%。CuMgLa/Al2O3 was prepared from Cu(NO3)2·3H2 O by coprecipitation method and characterized by TEM and N2 adsorption-desorption technique.The results showed that CuMgLa/Al2O3 had a mesoporous structure and the particle size of the main active component CuO was about 25 nm.The effects of temperature and catalyst mass concentration on the degradation of quinoline by wet catalytic oxidation were investigated.It was found that under the conditions of mass concentration of quinoline simulated wastewater 1000 mg/L,catalyst mass concentration 0.2 g/L,reaction temperature 240℃,oxygen partial pressure 0.53 MPa,reaction time 60 min,the removal rate of quinoline could reach about 100.0%,and the removal rate of chemical oxygen demand(COD)could reach 94.8%.The quenching experiment of tert-butanol revealed that·OH oxidation played a key role in quinoline degradation.The intermediate of quinoline degradation were analyzed by LC-MS and UV spectra,and the possible degradation path of quinoline was speculated.Meanwhile,under the optimal conditions,COD removal rate of 7000 mg/L mass concentration of simulated coking wastewater could reach 94.6%.The removal rates of COD and NH3-N were 69.6%and 28.0%for the actual coking wastewater with COD and NH3-N mass concentrations of 4740.0 and of 884.2 mg/L.

关 键 词：湿式催化氧化 喹啉 淬灭实验 降解路径 焦化废水 水处理技术 

分 类 号：TQ630[化学工程—精细化工]