煤化工高盐废水臭氧催化氧化脱除COD  

COD removal from high-salt wastewater in coal chemical industry by ozone catalytic oxidation

作　　者：马栋 段锋[3] MA Dong;DUAN Feng(Research Institute of Coal Chemistry,China Coal Research Institute,Beijing 100013,China;State Key Laboratory of High Efficient Mining and Clean Utilization of Coal Resources,China Coal Research Institute,Beijing 100013,China;Department of Environmental Technology and Engineering,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China)

机构地区：[1]煤炭科学技术研究院有限公司煤化工分院,北京100013 [2]煤炭资源高效开采与洁净利用国家重点实验室,北京100013 [3]中国科学院过程工程研究所环境技术与工程研究部,北京100190

出　　处：《环境工程学报》2020年第4期984-992,共9页Chinese Journal of Environmental Engineering

基　　金：中国煤炭科工集团科技创新基金资助项目(2018MS002)。

摘　　要：针对煤化工高盐废水中有机物难降解问题,采用浸渍-煅烧法制备了负载有活性金属氧化物的活性氧化铝型催化剂,探索催化剂的制备工艺和反应操作条件对废水COD去除率的影响。结果表明:活性氧化铝载体催化性能优于陶粒,活性氧化铝负载Cu、Mn、Ni的催化活性较高,将2种活性组分进行组合制得的MnOxNiOx/γ-Al2O3催化剂,在经过60 min的臭氧催化氧化后,COD的去除率可达51.3%;利用BET、SEM-EDS、XRD对催化剂进行了表征和分析,Mn、Ni成功负载到活性氧化铝表面和孔隙内,2种元素负载量摩尔比约为2:1,且主要以氧化物形式存在;通过计算臭氧利用效率,发现MnOx-NiOx/γ-Al2O3臭氧催化氧化的η值低于单独的臭氧氧化,这意味着通过MnOx-NiOx/γ-Ak2O3催化剂可以有效地将臭氧分解成活性氧;通过优化臭氧和催化剂投加量后发现,在臭氧为350 mg·(L·h)-1、催化剂投加量为100 g·L-1废水中,反应180 min后,COD去除率可达到72.3%;在连续进行4 h的臭氧催化氧化实验后,MnOx-NiOx/γ-Al2O3稳定性和重复利用性均较好,COD去除率能维持在约42%,锰、镍离子的溶出量均小于0.5 mg·L-1。以上研究结果可为高效的臭氧催化体系在煤化工高盐废水处理领域的应用提供参考。Aiming at the problem of refractory degradation of organic matters in high-salt wastewater from coal chemical industry,an active alumina-type catalyst loaded with active metal oxide was prepared by an impregnation-calcination method.The effects of catalyst preparation and reaction conditions on COD removal rate from wastewater were investigated.The experimental results showed that the catalytic performance of activated alumina carrier was better than that of ceramsite,and activated alumina supported with Cu,Mn,Ni had high catalytic activity,of which the MnOx-NiOx/γ-Al2O3 catalyst prepared by the combination of the two active components could catalyze the ozone oxidation reaction with 51.3% COD removal after 60 minutes.The catalyst was characterized and analyzed by BET,SEM-EDS,XRD.The results showed that Mn,Ni elements were successfully loaded on the surface and pores of activated alumina,and their molar ratio was about 2:1,and their oxide forms mainly appeared.Through calculating the ozone utilization efficiency,the η value of the MnOx-NiOx/γ-Al2O3 catalyst was lower than that of ozone alone.This implied that the MnOx-NiOx/γ-Al2O3 catalyst could effectively decompose ozone into ROS.After optimizing the dosage of ozone and the dosage of the catalyst,the optimum dosages of catalyst and ozone were 100 g·L-1 and 350 mg·(L·h)-1,respectively,at which the COD removal rate could reach 72.3% after 180 min reaction.After 4 hours ozone catalytic oxidation,the stability and reusability of MnOx-NiOx/γ-Al2O3 were good,COD removal rate maintained about 42% and the release amounts of manganese and nickel ions were less than 0.5 mg·L-1.This study can provide a reference for the development of an efficient ozone catalytic system and its application in the field of high-salt wastewater treatment in the coal chemical industry.

关 键 词：煤化工高盐废水 MnOx-NiOx/γ-Al2O3催化剂 COD去除率 臭氧催化氧化 

分 类 号：X703[环境科学与工程—环境工程]