[發明專利]一種提高四酰胺基六甲基苯基環鐵反應活性的復合材料及其制備方法和應用方法

有效

• 申請號: 201710699627.4
• 申請日: 2017-08-15
• 公開（公告）號: CN107497487B
• 公開（公告）日: 2019-10-25
• 發明（設計）人: 谷成;王超
• 申請（專利權）人: 南京大學
• 主分類號: B01J31/22
• 分類號: B01J31/22;B01J20/20;B01J20/30;C02F1/72;C02F101/36
• 代理公司: 江蘇瑞途律師事務所 32346
• 代理人: 蔣海軍

本發明公開了一種提高四酰胺基六甲基苯基環鐵(Fe(III)?TAML)反應活性的復合材料及其制備方法和應用方法，屬于環境功能材料合成領域，解決了Fe(III)?TAML在中性或近中性條件下反應活性顯著降低的問題。本發明以二氯甲烷/水混合溶劑為媒介，以全氟辛酸PFOA作為摻雜劑，通過表面活性劑雙十八烷基二甲基氯化銨(DODMA)輔助自組裝的方法合成了以Fe(III)?TAML為基底的微觀復合材料Fe(III)?TAML/DODMA/PFOA，與現有技術的游離態Fe(III)?TAML相比較，通過表面活性劑輔助自組裝合成的復合材料Fe(III)?TAML/DODMA/PFOA的反應活性顯著提高。

技術領域

本發明屬于環境功能材料合成領域，更具體地說，涉及一種提高四酰胺基六甲基苯基環鐵反應活性的復合材料及其制備方法和應用方法。

背景技術

過氧化氫活化劑四酰胺基六甲基苯基環鐵(簡稱四酰胺環鐵，Fe(III)-TAML)能夠高效去除多種有機污染物，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)、有機磷農藥殺螟硫磷(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)、危險的細菌孢子(D.Banerjee,A.L.Markley,et al.,“Green”Oxidation Catalysis for RapidDeactivation of Bacterial Spores,Angewandte Chemie International Edition 45(2006)3974-3977)、藥物成分舍曲林(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)以及炸藥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的活性具有很強的pH依賴性，會在中性和酸性條件下顯著降低(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)。