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基于固载聚铌酸盐的多功能自解毒材料用于化学战剂模拟物的净化。

A Versatile Self-Detoxifying Material Based on Immobilized Polyoxoniobate for Decontamination of Chemical Warfare Agent Simulants.

机构信息

Key Laboratory of Cluster Science Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic, Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081, P. R. China.

出版信息

Chemistry. 2018 Dec 20;24(72):19208-19215. doi: 10.1002/chem.201804523. Epub 2018 Dec 10.

Abstract

A decontaminating composite, Mg Al-LDH-Nb , has been successfully prepared by immobilizing Lindqvist [H Nb O ] (Nb ) into a Mg Al-based layered double hydroxide (Mg Al-LDH). To our knowledge, this represents the first successful approach to the immobilization of polyoxoniobate. As a versatile catalyst, Mg Al-LDH-Nb can effectively catalyze the degradation of both vesicant and nerve agent simulants by multiple pathways under mild conditions. Specifically, the sulfur mustard simulant, 2-chloroethyl ethyl sulfide (CEES), is converted into the corresponding nontoxic 2-chloroethyl ethyl sulfoxide (CEESO) by selective oxidation, whereas the Tabun (G-type nerve agent) simulant, diethyl cyanophosphonate (DECP), and the VX (V-type nerve agent) simulant, O,S-diethyl methylphosphonothioate (OSDEMP), are detoxified through hydrolysis and perhydrolysis, respectively. A possible mechanism is proposed on the basis of control experiments and spectroscopic studies. The Mg Al-LDH-Nb composite exhibits remarkable robustness and can be readily reused for up to ten cycles with negligible loss of its catalytic activity. More importantly, a protective "self-detoxifying" material has easily been constructed by integrating Mg Al-LDH-Nb into textiles. In this way, the flexible and permeable properties of textiles have been combined with the catalytic activity of polyoxoniobate to remove 94 % of CEES in 1 h by using nearly stoichiometric dilute H O (3 %) as oxidant with 96 % selectivity.

摘要

一种去污复合材料 Mg Al-LDH-Nb 已成功制备,其方法是将 Lindqvist [H Nb O ](Nb )固定在 Mg Al 基层状双氢氧化物(Mg Al-LDH)中。据我们所知,这代表了多氧代铌化合物固定化的首次成功尝试。作为一种多功能催化剂,Mg Al-LDH-Nb 在温和条件下可通过多种途径有效催化两种糜烂性毒剂和神经性毒剂模拟物的降解。具体而言,硫芥模拟物 2-氯乙基乙基硫醚(CEES)通过选择性氧化转化为相应的无毒 2-氯乙基乙基砜(CEESO),而沙林(G 型神经性毒剂)模拟物二乙基氰膦酸酯(DECP)和维埃克斯(V 型神经性毒剂)模拟物 O,S-二乙基甲基膦酸硫酯(OSDEMP)则通过水解和过水解分别解毒。基于对照实验和光谱研究提出了一种可能的机制。Mg Al-LDH-Nb 复合材料表现出显著的稳定性,可重复使用多达十次,催化活性几乎没有损失。更重要的是,通过将 Mg Al-LDH-Nb 整合到纺织品中,很容易构建一种具有“自我解毒”功能的防护材料。通过使用近化学计量的稀 H O(3%)作为氧化剂,纺织品的柔性和透气性与多氧代铌化合物的催化活性相结合,在 1 h 内可去除 94%的 CEES,选择性达到 96%。

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