Recoverable amphiphilic polyoxoniobates catalyzing oxidative and hydrolytic decontamination of chemical warfare agent simulants in emulsion
Recoverable amphiphilic polyoxoniobates catalyzing oxidative and hydrolytic decontamination of chemical warfare agent simulants in emulsion
复制标题
可回收的两亲性聚氧铌酸盐催化乳液中化学战剂模拟物的氧化和水解净化
DOI：
10.1016/j.jhazmat.2017.11.061
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发表时间：
2018
期刊：
影响因子：
--
通讯作者：
Hu Changwen
中科院分区：
文献类型：
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作者：
Li Xiaoqin;Dong Jing;Liu Huifang;Sun Xiangrong;Chi Yingnan;Hu Changwen
通过己酸阴离子与含长烷基链季铵的静电相互作用，成功制备了两亲性多氧氧酸盐（PONbs） [CnH2n+1N(CH3)3]7HNb6O19(for1, n = 14; for2, n = 16; for3, n = 18)，并利用傅里叶变换红外（FT-IR）、1H核磁共振（1H NMR）、13C核磁共振（13C NMR）、热重分析（TGA）和元素分析等多种技术对其进行了表征。将这三种PONbs用于乳液体系中对化学战剂模拟物的催化净化，并评价了季铵盐阳离子、聚阴离子和催化剂用量对催化效率的影响。在最佳条件下，催化剂乳液可以在2小时内水解完全转化神经毒剂模拟物二乙基氰膦酸酯（DECP），并在20分钟内用接近化学量的3% H2O2水溶液氧化完全转化芥子气模拟物2-氯乙基硫醚（CEES）。此外，两亲性催化剂可以很容易地分离并重复使用五次，而不会明显失去其活性。据我们所知，这项研究是第一个使用PONbs乳液进行催化的例子。
Amphiphilic polyoxoniobates (PONbs), [CnH2n+1N(CH3)3]7HNb6O19(for1, n = 14; for2, n = 16; and for3, n = 18), were successfully prepared by the electrostatic interaction of hexaniobate anions with quaternary ammoniums containing long alkyl chain, and thoroughly characterized by using various techniques including Fourier transform infrared (FT-IR),1H nuclear magnetic resonance (1H NMR),13C nuclear magnetic resonance (13C NMR), thermogravimetric analysis (TGA), and elemental analysis. All three PONbs were used in the emulsion systems to catalytically decontaminate chemical warfare agent simulants and the influences of quaternary ammonium cations, polyanions, and amount of catalyst on the catalytic efficiency have been evaluated. Under optimal conditions, catalyst3in emulsion can completely convert both a the nerve agent simulant, diethyl cyanophosphonate (DECP), in 2 h by hydrolysis and a sulfur mustard simulant, 2-chloroethyl ethyl sulfide (CEES), in 20 min by oxidation using nearly stoichiometric 3% aqueous H2O2. Moreover, the amphiphilic catalyst3can be simply separated and readily reused for five recycles without obvious losing its activity. To the best of our knowledge, this study represents the first example where the emulsions of PONbs are used in the catalysis.