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    李佳怿, 孙贤波, 刘勇弟. N-117负载Fe(Ⅱ)非均相芬顿体系催化降解对氯苯酚[J]. 华东理工大学学报(自然科学版), 2018, 44(6): 855-861. DOI: 10.14135/j.cnki.1006-3080.20180110003
    引用本文: 李佳怿, 孙贤波, 刘勇弟. N-117负载Fe(Ⅱ)非均相芬顿体系催化降解对氯苯酚[J]. 华东理工大学学报(自然科学版), 2018, 44(6): 855-861. DOI: 10.14135/j.cnki.1006-3080.20180110003
    LI Jia-yi, SUN Xian-bo, LIU Yong-di. Catalytic Degradation of p-Chlorophenol by N-117 Supported Fe (Ⅱ) Catalyzed Heterogeneous Fenton Reaction[J]. Journal of East China University of Science and Technology, 2018, 44(6): 855-861. DOI: 10.14135/j.cnki.1006-3080.20180110003
    Citation: LI Jia-yi, SUN Xian-bo, LIU Yong-di. Catalytic Degradation of p-Chlorophenol by N-117 Supported Fe (Ⅱ) Catalyzed Heterogeneous Fenton Reaction[J]. Journal of East China University of Science and Technology, 2018, 44(6): 855-861. DOI: 10.14135/j.cnki.1006-3080.20180110003

    N-117负载Fe(Ⅱ)非均相芬顿体系催化降解对氯苯酚

    Catalytic Degradation of p-Chlorophenol by N-117 Supported Fe (Ⅱ) Catalyzed Heterogeneous Fenton Reaction

    • 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300 min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100 mg/L,反应20 min,对氯苯酚降解率可达95.6%,溶出总铁质量浓度为0.67 mg/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0~500 mg/L内升高时,反应60 min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25 mg/L时,反应60 min溶出总铁质量浓度由0.67 mg/L升高至9.4 mg/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。

       

      Abstract: Iron loaded N-117 Nafion membrane has been proved to be an efficient and stable heterogeneous Fenton catalyst. In this paper, Fe(Ⅱ) loaded N-117 was 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-117 can 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 was 9.0, p-chlorophenol degradation rate was 87.3% within 300 min. Catalytic reaction rate decreased as the initial pH was increased. When initial pH was 3.0 and H2O2 mass concentration was 100 mg/L, p-chlorophenol degradation rate was 95.6% within 20 min, with dissolved Fe mass concentration being limited to 0.67 mg/L. When H2O2 mass concentration exceeded 100 mg/L, the rate of p-chlorophenol catalytic degradation did not go up with H2O2 mass concentration and it was limited by ferryl concentration and mass transfer. As chloride mass concentration increased from 0 to 500 mg/L, p-chlorophenol degradation rate remained no less than 87.0% within 60 min 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 from 0 to 25 mg/L, p-chlorophenol degradation rate remained no less than 90.2% within 60 min. Total dissolution of Fe increased from 0.67 mg/L to 9.4 mg/L, while total amount of Fe dissolution was only 4.7%. Fe clusters were observed on the surface of the used N-117, but the membrane skeleton was not destroyed by oxidation.

       

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