催化学报

催化学报 ›› 2016, Vol. 37 ›› Issue (1): 135-145.DOI: 10.1016/S1872-2067(15)61010-5

• 论文 • 上一篇    下一篇

封装Fe(III),Ni(II)和Cu(II)的N,N'-双邻羟苯亚甲基-1,2-苯二胺络合物的Y分子筛催化4-氯-3-甲基苯酚氧化反应

Solomon Legese Hailua,b, Balachandran Unni Naira, Mesfin Redi-Abshirob, Isabel Diazb,c, Rathinam Aravindhana, Merid Tessemab   

  1. a 中央皮革研究所化工实验室, 金奈600 020, 阿达亚, 印度;
    b 亚的斯亚贝巴大学化学系, 亚的斯亚贝巴1176, 埃塞俄比亚;
    c 催化与石油化学研究所, 康都布兰戈28049, 马德里, 西班牙
  • 收稿日期:2015-08-11 修回日期:2015-11-06 出版日期:2015-12-26 发布日期:2015-12-26
  • 通讯作者: Balachandran Unni Nair
  • 作者简介:Balachandran Unni Nair

Oxidation of 4-chloro-3-methylphenol using zeolite Y-encapsulated iron(III)-, nickel(II)-, and copper(II)-N,N'-disalicylidene- 1,2-phenylenediamine complexes

Solomon Legese Hailua,b, Balachandran Unni Naira, Mesfin Redi-Abshirob, Isabel Diazb,c, Rathinam Aravindhana, Merid Tessemab   

  1. a Chemical Laboratory, CSIR-Central Leather Research Institute, Adyar, Chennai 600 020, India;
    b Department of Chemistry, Addis Ababa University, P.O. Box 1176, Addis Ababa, Ethiopia;
    c Instituto de Catálisis y Petroleoquímica, ICP-CSIC, C/Marie Curie 2, 28049 Cantoblanco, Madrid, Spain
  • Received:2015-08-11 Revised:2015-11-06 Online:2015-12-26 Published:2015-12-26
  • Contact: Balachandran Unni Nair

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摘要：

将Fe(III), Ni(III)和Cu(II)与N,N'-双邻羟苯亚甲基-1,2-苯二胺配位的络合物封装在Y分子筛内,作为多相类Fenton的高级氧化过程的催化剂,用于降解4-氯-3-甲基苯酚(PCMC).采用粉末X射线衍射、热重、N2吸附-脱附、红外光谱、元素分析和扫描电镜对所制催化剂的物化性质进行了表征,并考察了H2O2的初始浓度、催化剂用量、温度和pH值等因素对模型有机污染物降解的影响.结果表明,在Fe(III),Ni(III)和Cu(II)催化剂作用下,在较低的酸性pH值、催化剂用量0.1g、H2O2的初始浓度0.35mmol/L的条件下,于50℃反应120min几乎可以完全去除PCMC.同时还考察了所制PCMC降解催化剂的重复使用性能,提出了可能的催化剂失活机理,也研究了PCMC氧化过程中可能的中间产物和动力学.

关键词: 瓶中造船法, 4-氯-3-甲基苯酚, 拟一级反应, 失活, 羟基自由基

Abstract:

The degradation of 4-chloro-3-methylphenol (PCMC) using zeolite-encapsulated iron(III), nickel(II), and copper(II) complexes of N,N'-disalicylidene-1,2-phenylenediamine as catalysts, in a heterogeneous Fenton-like advanced oxidation process, was studied. The physicochemical properties of the catalysts were determined using powder X-ray diffraction, thermogravimetric analysis, Brunauer-Emmett-Teller surface area analysis, Fourier-transform infrared spectroscopy, elemental analysis, and scanning electron microscopy. The effects of four factors, namely initial H2O2 concentration, catalyst dosage, temperature, and pH, on the degradation of a model organic pollutant were determined. The results show that at low acidic pH, almost complete removal of PCMC was achieved with the iron(III), nickel(II), and copper(II) catalysts after 120 min under the optimum reaction conditions: catalyst dosage 0.1 g, H2O2 concentration 75 mmol/L, initial PCMC concentration 0.35 mmol/L, and 50 ℃. The reusability of the prepared catalysts in PCMC degradation was also studied and a possible catalyst deactivation mechanism is proposed. The possible intermediate products, degradation pathway, and kinetics of PCMC oxidation were also studied.

Key words: Ship-in-a-bottle method, 4-Chloro-3-methylphenol, Pseudo-first order, Deactivation, Hydroxyl radical