MnCeO_(x)催化湿式氧化处理丙烯腈废水  

Study on catalytic wet air oxidation of acrylonitrile wastewater over MnCeO_(x)

作　　者：陈航宁 许丹丹 郑育元 杜辰昊 吴粮华 刘红星 CHEN Hangning;XU Dandan;ZHENG Yuyuan;DU Chenhao;WU Lianghua;LIU Hongxing(Sinopec Shanghai Research Institute of Petrochemical Technology CO.,Ltd.,Shanghai 201208,China)

机构地区：[1]中石化(上海)石油化工研究院有限公司,上海201208

出　　处：《化工环保》2024年第4期511-516,共6页Environmental Protection of Chemical Industry

摘　　要：采用柠檬酸络合法制备了系列MnCeO_(x)催化剂,运用SEM、TEM、XRD和H_(2)-TPR等技术对其进行了表征,并将MnCeO_(x)应用于催化湿式氧化处理丙烯腈废水,考察了Mn与Ce的摩尔比、焙烧温度、反应温度等因素对处理效果的影响。结果表明:当Mn与Ce的摩尔比为7∶3、焙烧温度为500℃时,所制备的Mn_(0.7)Ce_(0.3)O_(x)催化剂活性最好,当pH 7.00、反应温度250℃、反应时间1 h时,丙烯腈废水经催化湿式氧化处理后,COD去除率为95.5%,BOD_(5)/COD从0.04提高至0.65,总氰质量浓度从9.10 mg/L降低至0.06 mg/L,去除率为99.3%;当反应温度250℃、压力7 MPa、丙烯腈废水pH 7.00、进水流量1 mL/min、停留时间1 h时,Mn_(0.7)Ce_(0.3)O_(x)在连续运行500 h后,活性组分Mnn+的质量分数从41.17%降至40.90%,COD去除率稳定在90%以上,表现出良好的活性和稳定性。A series of MnCeO_(x)catalysts were prepared by the citric acid complexation method,and applied to treat acrylonitrile wastewater through catalytic wet oxidation(CWO).The catalysts were characterized by SEM,TEM,XRD,and H_(2)-TPR technologies.The effects of the factors,including the molar ratio of Mn to Ce,calcination temperature,and reaction temperature,on the treatment efficiency were investigated.The results showed that the best activity of the prepared Mn_(0.7)Ce_(0.3)O_(x)catalyst occurs when the molar ratio of Mn to Ce was 7∶3 and the calcination temperature was 500℃.During the batch reaction,when the reaction condition of 250℃,pH 7.00,after 1 h CWO treatment of acrylonitrile wastewater,the COD removal rate is 95.5%,BOD_(5)/COD increased from 0.04 to 0.65,and the total cyanide mass concentration decreased from 9.10 mg/L to 0.06 mg/L,with a removal rate of 99.3%.In the continuous reaction,Mn_(0.7)Ce_(0.3)O_(x)shows excellent activity and stability.After continuous reaction for 500 h at 250℃,7 MPa,pH 7.00,the influent flow rate of 1 mL/min,and residence time of 1 h,Mnn+slightly decreased from 41.17%(w)to 40.90%(w),and the COD removal rate of acrylonitrile wastewater remained stable above 90%.

关 键 词：催化湿式氧化 丙烯腈废水 MnO_(2) CeO_(2) 复合氧化物 

分 类 号：X783.4[环境科学与工程—环境工程]