封装Fe(III),Ni(II)和Cu(II)的<i>N</i>,<i>N</i>'-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

引用本文: Solomon Legese Hailu, Balachandran Unni Nair, Mesfin Redi-Abshiro, Isabel Diaz, Rathinam Aravindhan, Merid Tessema. 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[J]. 催化学报, 2016, 37(1): 135-145. doi: 10.1016/S1872-2067(15)61010-5 shu

Citation: Solomon Legese Hailu, Balachandran Unni Nair, Mesfin Redi-Abshiro, Isabel Diaz, Rathinam Aravindhan, Merid Tessema. Oxidation of 4-chloro-3-methylphenol using zeolite Y-encapsulated iron(III)-, nickel(II)-, and copper(II)-N,N'-disalicylidene- 1,2-phenylenediamine complexes[J]. Chinese Journal of Catalysis, 2016, 37(1): 135-145. doi: 10.1016/S1872-2067(15)61010-5 shu

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

1.
a 中央皮革研究所化工实验室, 金奈600 020, 阿达亚, 印度;
2.
b 亚的斯亚贝巴大学化学系, 亚的斯亚贝巴1176, 埃塞俄比亚;
3.
c 催化与石油化学研究所, 康都布兰戈28049, 马德里, 西班牙

通讯作者: Balachandran Unni Nair

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:

English

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

1.
a Chemical Laboratory, CSIR-Central Leather Research Institute, Adyar, Chennai 600 020, India;
2.
b Department of Chemistry, Addis Ababa University, P.O. Box 1176, Addis Ababa, Ethiopiac Instituto de Catálisis y Petroleoquímica, ICP-CSIC, C/Marie Curie 2, 28049 Cantoblanco, Madrid, Spain

Corresponding author: Balachandran Unni Nair

Received Date: 11 August 2015

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:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

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

通讯作者: Balachandran Unni Nair

English

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

Corresponding author: Balachandran Unni Nair

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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

通讯作者: Balachandran Unni Nair

English

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

Corresponding author: Balachandran Unni Nair

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

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