[发明专利]一种提高四酰胺基六甲基苯基环铁反应活性的复合材料及其制备方法和应用方法

说明书

本发明公开了一种提高四酰胺基六甲基苯基环铁(Fe(III)‑TAML)反应活性的复合材料及其制备方法和应用方法，属于环境功能材料合成领域，解决了Fe(III)‑TAML在中性或近中性条件下反应活性显著降低的问题。本发明以二氯甲烷/水混合溶剂为媒介，以全氟辛酸PFOA作为掺杂剂，通过表面活性剂双十八烷基二甲基氯化铵(DODMA)辅助自组装的方法合成了以Fe(III)‑TAML为基底的微观复合材料Fe(III)‑TAML/DODMA/PFOA，与现有技术的游离态Fe(III)‑TAML相比较，通过表面活性剂辅助自组装合成的复合材料Fe(III)‑TAML/DODMA/PFOA的反应活性显著提高。

技术领域

本发明属于环境功能材料合成领域，更具体地说，涉及一种提高四酰胺基六甲基苯基环铁反应活性的复合材料及其制备方法和应用方法。

背景技术

过氧化氢活化剂四酰胺基六甲基苯基环铁(简称四酰胺环铁，Fe(III)-TAML)能够高效去除多种有机污染物，如氯酚(S.S.Gupta,M.Stadler,et al.,Rapid TotalDestruction of Chlorophenols by Activated Hydrogen Peroxide,Science 296(2002)326-328；K.Mierzwicki,S.Berski,et al.,AIM and ELF analysis of the H-,Me-,andF-substituted FeIII–TAML complexes,Chemical Physics Letters 507(2011)29-36)、有机磷农药杀螟硫磷(A.Chanda,S.K.Khetan,et al.,Total Degradation ofFenitrothion and Other Organophosphorus Pesticides by Catalytic OxidationEmploying Fe-TAML Peroxide Activators,Journal of the American ChemicalSociety128(2006)12058-12059)、二苯并噻吩(S.Mondal,Y.Hangun-Balkir,et al.,Oxidation of sulfur components in diesel fuel using Fe-catalysts andhydrogen peroxide,Catalysis Today 116(2006)554-561)、天然和合成的雌激素(N.W.Shappell,M.A.Vrabel,et al.,Destruction of Estrogens Using Fe-TAML/Peroxide Catalysis,Environmental Science&Technology 42(2008)1296-1300)，偶氮燃料(N.Chahbane,D.L.Popescu,et al.,FeIII-TAML-catalyzed green oxidativedegradation of the azo dye Orange II by H₂O₂and organic peroxides：products,toxicity,kinetics,and mechanisms,Green Chemistry 9(2007)49-57)、危险的细菌孢子(D.Banerjee,A.L.Markley,et al.,“Green”Oxidation Catalysis for RapidDeactivation of Bacterial Spores,Angewandte Chemie International Edition 45(2006)3974-3977)、药物成分舍曲林(L.Q.Shen,E.S.Beach,et al.,Rapid,BiomimeticDegradation in Water of the Persistent Drug Sertraline by TAML Catalysts andHydrogen Peroxide,Environmental Science&Technology 45(2011)7882-7887)以及炸药TNT和TNB(S.Kundu,A.Chanda,et al.,TAML Activator/Peroxide-Catalyzed FacileOxidative Degradation of the Persistent Explosives Trinitrotoluene andTrinitrobenzene in Micellar Solutions,Environmental Science&Technology 47(2013)5319-5326)。Fe(III)-TAML的活性具有很强的pH依赖性，会在中性和酸性条件下显著降低(V.Polshin,D.L.Popescu,et al.,Attaining Control by Design over theHydrolytic Stability of Fe-TAML Oxidation Catalysts,Journal of the AmericanChemical Society 130(2008)4497-4506；D.L.Popescu,A.Chanda,et al.,Mechanistically Inspired Design of FeIII-TAML Peroxide-Activating Catalysts,Journal of the American Chemical Society130(2008)12260-12261)。