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N-117负载Fe(Ⅱ)非均相芬顿体系催化降解对氯苯酚 被引量:4

Catalytic Degradation of p-Chlorophenol by N-117 Supported Fe(Ⅱ)Catalyzed Heterogeneous Fenton Reaction
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摘要 N-117负载铁催化剂能有效催化芬顿反应,铁溶出率低。采用N-117负载非均相芬顿体系催化降解对氯苯酚,研究了初始pH、过氧化氢质量浓度、氯离子质量浓度和腐殖酸质量浓度对对氯苯酚去除效率和催化剂稳定性的影响。结果表明:N-117负载Fe(Ⅱ)催化剂能有效催化降解对氯苯酚,拓宽芬顿反应使用pH范围,降低氯离子催化芬顿反应的抑制效果。当初始pH=9.0时,反应300min对氯苯酚降解率可达87.3%。随着初始pH升高,催化反应速率下降。过氧化氢初始质量浓度为100mg/L,反应20min,对氯苯酚降解率可达95.6%,溶出总铁质量浓度为0.67mg/L;过氧化氢继续增多时,受到高价铁基团和传质速率的限制,对氯苯酚降解速率不随过氧化氢质量浓度升高而加快。氯离子质量浓度在0~500mg/L内升高时,反应60min对氯苯酚降解率能达到87.0%以上,但铁的溶出显著增加,对氯苯酚降解速率减慢。腐殖酸质量浓度由0升高到25mg/L时,反应60min溶出总铁质量浓度由0.67mg/L升高至9.4mg/L,总铁溶出率不高于4.7%,对氯苯酚降解率仍能达到90.2%以上。催化剂使用后负载铁发生团聚,但膜骨架未被氧化破坏。 Iron loaded N-117Nafion membrane has been proved to be an efficient and stable heterogeneous Fenton catalyst.In this paper,Fe(Ⅱ)loaded N-117was used to catalyze Fenton reaction and p-chlorophenol degradation.The influences of initial pH,hydrogen peroxide concentration,chlorine and humic acid on its catalytic activity and stability were investigated.Fe(Ⅱ)loaded N-117can effectively catalyze p-chlorophenol degradation,increase the pH range for Fenton reaction,and reduce the inhibition of chloride ion on p-chlorophenol degradation.When initial pH was9.0,p-chlorophenol degradation rate was87.3%within300min.Catalytic reaction rate decreased as the initial pH was increased.When initial pH was3.0and H2O2mass concentration was100mg/L,p-chlorophenol degradation rate was95.6%within20min,with dissolved Fe mass concentration being limited to0.67mg/L.When H2O2mass concentration exceeded100mg/L,the rate of p-chlorophenol catalytic degradation did not go up with H2O2mass concentration and it was limited by ferryl concentration and mass transfer.As chloride mass concentration increased from0to500mg/L,p-chlorophenol degradation rate remained no less than87.0%within60min reaction time.However,p-chlorophenol degradation rate was decreased,and the dissolution rate of Fe was enhanced.When the mass concentration of humic acid was increased from0to25mg/L,p-chlorophenol degradation rate remained no less than90.2%within60min.Total dissolution of Fe increased from0.67mg/L to9.4mg/L,while total amount of Fe dissolution was only4.7%.Fe clusters were observed on the surface of the used N-117,but the membrane skeleton was not destroyed by oxidation.
作者 李佳怿 孙贤波 刘勇弟 LI Jia-yi;SUN Xian-bo;LIU Yong-di(School of Resources and Environmental Engineering,East China University ofScience and Technology,Shanghai 200237,China)
出处 《华东理工大学学报(自然科学版)》 CAS CSCD 北大核心 2018年第6期855-861,共7页 Journal of East China University of Science and Technology
关键词 非均相芬顿 对氯苯酚 氯离子 腐殖酸 heterogeneous Fenton p-chlorophenol chloride ion humic acid
作者简介 李佳怿(1993-),女,山东省济南人,硕士生,研究方向为废污水处理的高价氧化技术。E-mail:leslie_lijiayi@sina.com;通信联系人:刘勇弟,E-mail:ydliu@ecust.edu.cn
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