Fe_2O_3微纳米材料对八氯萘的热催化降解及其机制研究  

Catalytic thermal degradation of octachloronaphthalene over Fe_2O_3 micro/nanomaterial and its explored mechanism

作　　者：赵彦辉[1,2] 芦会杰[2] 徐文[1] 黄林艳[2] 李倩倩[2] 李宾克 黄鑫辰 苏贵金[2] 

机构地区：[1]海南大学,环境与植物保护学院,海口570100 [2]中国科学院生态环境研究中心,环境化学与生态毒理学国家重点实验室,北京100085

出　　处：《环境化学》2015年第12期2204-2212,共9页Environmental Chemistry

基　　金：国家重点基础研究发展规划(973)项目(2015CB453103);国家自然科学基金(21377147,21177141,21321004)资助

摘　　要：本文研究了制备的α-Fe_2O_3微/纳米材料对八氯萘(octachloronaphthalene,CN-75)的催化降解活性及降解机制.在300℃下动力学研究发现,α-Fe_2O_3降解CN-75的反应行为呈现准一级动力学反应特征,反应速率常数为0.075 min^(-1).在α-Fe_2O_3催化下CN-75能够发生逐级加氢脱氯反应,生成一系列的七氯至二氯萘产物,且初始加氢脱氯优先发生在α位.此外,CN-75还能发生氧化开环反应生成甲酸、乙酸等中间产物.根据检测到的降解产物推测CN-75在α-Fe_2O_3上的降解反应历程为:CN-75→CN-73→CN-66/67→CN-54、CN-52、CN-51、CN-50→……→HCOOH+CH_3COOH.Degradation of octachloronaphthalene（ CN-75） was performed over as-prepared α-Fe_2O_3 micro / nano materials. The degradation process conforms to the first order reaction kinetics with kobs=0.075 min^（-1） at 300 ℃. The identification of heptachloronaphthalene to dichloronaphthalene as the products indicates the occurrence of successive hydrodechlorination reactions during the degradation of CN-75 over the prepared α-Fe_2O_3. The Cl atom at α-position was removed preferentially theβ-position. Furthermore,the oxidative products,such as formic and acetic acids,were identified simultaneously,suggesting that CN-75 can be ring-cracked into small organic molecules. According to the identified products,the pathway for the degradation of CN-75 over α-Fe_2O_3 was speculated as the following： CN-75 → CN-73 → CN-66 / 67 → CN-54、CN-52、CN-51、CN-50 → …… → HCOOH ＋CH_3COOH.

关 键 词：CN-75 Α-FE2O3 FE3O4 逐级加氢脱氯 

分 类 号：X701[环境科学与工程—环境工程] O643.32[理学—物理化学]