Mn-Ce/ZSM-5催化剂在连续固定床反应器中催化湿式氧化苯酚废水  

Wet oxidation of phenol wastewater catalyzed by Mn-Ce/ZSM-5 catalyst in a fixed-bed reactor

作　　者：孙子凯 赵国峥[1] 李长波[1] 星大松 肖丽光 SUN Zikai;ZHAO Guozheng;LI Changbo;XING Dasong;XIAO Liguang(School of Environmental and Safety Engineering,Liaoning Petrochemical University,Fushun 113001,China;Engineering and Technology Research Center,Fushun Mining Group Co.,Ltd.,Fushun 113001,China)

机构地区：[1]辽宁石油化工大学环境与安全工程学院,抚顺113001 [2]抚顺矿业集团有限责任公司工程技术研究中心,抚顺113001

出　　处：《给水排水》2023年第5期66-73,共8页Water & Wastewater Engineering

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：采用溶胶凝胶法制备了Mn-Ce/ZSM-5催化剂,将其用于催化湿式过氧化氢氧化(CWPO)苯酚废水。考察了连续固定床反应器中负载量、反应温度、进料液流量对苯酚降解性能的影响,并测定了催化剂稳定性。结果表明,随反应温度增加,苯酚降解率升高;随进料液流量增加,苯酚降解率降低;随苯酚入口浓度增加,苯酚降解率降低。在pH=3、温度140℃、催化剂投加量1 g、进料液流量2 mL/min、苯酚浓度1000 mg/L、固定床连续运转3 h的条件下,COD去除率84.59%,一次再生催化剂连续处理5 L苯酚废水后,催化剂降解效率开始明显降低。XRD、BET、SEM和XPS的分析结果表明Mn-Ce/ZSM-5作为介孔催化剂,将Mn、Ce活性组分较好的负载在催化剂表面,能够有效的催化过氧化氢,将苯酚转化为邻苯二醌、对苯二醌等中间产物,最后完全氧化。Mn-Ce/ZSM-5 catalyst was prepared by sol-gel method and used to catalyze the wet hydrogen peroxide oxidation(CWPO)of phenol wastewater.The effects of loading,reaction temperature and feed liquid flow rate on the degradation performance of phenol in a continuous fixed bed reactor were investigated,and the stability of catalyst was measured.The results showed that the degradation rate of phenol increased with the increase of reaction temperature.The degradation rate of phenol decreases with the increase of feed liquid flow rate.The degradation rate of phenol decreased with the increase of phenol inlet concentration.Under the conditions of pH=3,temperature 140℃,catalyst dosage 1 g,feed liquid flow 2 mL/min,phenol concentration 1000 mg/L and continuous operation of the fixed bed for 3 h,the COD removal rate was 84.59%.After continuous treatment of 5 L phenol wastewater with a single regenerated catalyst,the degradation efficiency of catalyst began to decrease significantly..The results of XRD、BET、SEM and XPS showed that Mn-Ce/ZSM-5 was used as mesoporous catalyst,and the active components of Mn and Ce were well supported on the surface of the catalyst,which could effectively catalyze hydrogen peroxide,convert phenol into intermediate products such as adjacent benzoquinone and benzoquinone,and finally completely oxidize.

关 键 词：Mn-Ce/ZSM-5 CWPO 苯酚 固定床反应器 反应机理 

分 类 号：X703[环境科学与工程—环境工程]