碳纳米纤维增强钴酞菁催化氧化染料的性能研究  

Catalytic oxidation of dyes using carbon nanofiber to enhance the reactivity of cobalt phthalocyanine

作　　者：李楠[1] 卢琴[1] 高美萍[1] 吕汪洋[1] 姚玉元[1] 陈文兴[1] 

机构地区：[1]浙江理工大学材料与纺织学院,先进纺织材料与制备技术教育部重点实验室,杭州310018

出　　处：《中国科学：化学》2013年第6期774-782,共9页SCIENTIA SINICA Chimica

基　　金：国家自然科学基金(51133006;51103133;51003096);浙江省自然科学基金(Y4100094);浙江理工大学启动基金(1001803-Y)资助

摘　　要：将氨基钴酞菁(CoTAPc)以共价键的形式负载到碳纳米纤维(CNF)上制备碳纳米纤维负载钴酞菁催化剂(CoTAPc-CNF),利用原子吸收光谱、紫外-可见光吸收光谱、衰减全反射-红外光谱等方法对CoTAPc-CNF进行表征.选用具有氧杂蒽结构的罗丹明6G(Rh6G)为主要研究对象,研究CoTAPc-CNF对Rh6G的催化氧化性能,考察了温度、pH、NaCl、异丙醇等对CoTAPc-CNF催化性能的影响.结果表明,CoTAPc-CNF在常温中性条件下能有效催化氧化Rh6G;随着温度和pH的增加,CoTAPc-CNF催化氧化Rh6G速率逐渐提高;NaCl和异丙醇的加入,没有抑制催化氧化反应的进行,相反大大提高了Rh6G的降解速率,这与一般羟基自由基占主导的高级氧化体系完全不同;进一步采用电子顺磁共振波谱法证实CoTAPc-CNF/H2O2体系确实为非羟基自由基催化机理.另外,研究发现CoTAPc-CNF还能有效催化氧化其他共轭结构的染料,如偶氮染料酸性橙7(AO7)、三芳甲烷染料碱性绿1(BG1).因此,本文探索的CoTAPc-CNF/H2O2非羟基自由基催化反应体系在处理成分复杂的实际印染废水中具有较好的应用前景.Carboxylic acid-functionalized CNF was used to attach cobalt tetraaminophthalocyanine （CoTAPc） by amide bonds for obtaining carbon nanofiber-supported cobalt phthalocyanine （CoTAPc-CNF）. This catalyst was characterized by atomic absorption spectrometry, UV-vis spectroscopy, ATR-FTIR spectroscopy. The catalytic performance of CoTAPc-CNF was investigated by the oxidative degradation of Rhodamine 6G （Rh6G） with xanthine structure, and the effects of various conditions including temperature, pH, the addition of NaC1 and isopropanol were discussed. The results indicated that CoTAPc-CNF has a higher catalytic activity for the oxidation of dye at room temperature in neutral aqueous solution. The catalytic activity was raised with the increasing of temperature and pH. Moreover, the efficiency of Rh6G oxidation was improved while NaC1 or isopropanol was presented in this reaction system. This phenomenon was different from some common AOPs, in which chloride ion and isopropanol might serve as scavenger for hydroxyl radicals to inhibit the oxidation of dyes. EPR spin trapping technique indeed showed that the hydroxyl radical is not the major intermediate in the presence of CoTAPc-CNF. In addition, two different types of dyes including azo Acid Orange 7 （AO7） and triphenylmethane Basic Green 1 （BG1） could be also effectively degraded. This study provides a new idea for exploring the catalytic system with non-hydroxyl radical mechanism for the treatment of real wastewaters.

关 键 词：碳纳米纤维 钴酞菁 催化氧化 染料 

分 类 号：X703[环境科学与工程—环境工程]