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Oxidative Detoxification of Nerve Agent VX Simulant by Polyoxoniobate: Experimental and Theoretical Insights
Journal of Catalysis ( IF 6.5 ) Pub Date : 2021-01-05 , DOI: 10.1016/j.jcat.2020.12.029
Jing Dong , Xiangrong Sun , Ni Zhen , Zhen Li , Dan Liu , Bo Zou , Qipu Dai , Yingnan Chi , Shi-Lu Chen , Josep M. Poblet , Changwen Hu

VX is a representative nerve agent and its rapid detoxification relays on the development of catalysts and understanding of the mechanism on an atomic level. Herein, we report that a Lindqvist-type [Nb6O19]8- (Nb6) can effectively catalyze the detoxification of VX simulant, OSDEMP. Within 5 min OSDEMP can be completely converted to the minimally toxic product in the presence of H2O2. Various experimental evidences: (1) negligible conversion of DMNP (an organophosphorus ester without S center); (2) effect of solvent polarity; (3) 18O-labeled experiment confirm that the detoxification of OSDEMP by Nb6 follows an oxidation pathway. Further experimental and theoretical studies (e.g. spectroscopic analysis, control experiments, kinetic studies, and DFT calculations, etc.) reveal that Nb(ƞ1-OOH) hexaniobate is the dominant active species and both the formation of Nb(ƞ1-OOH) hexaniobate species and oxygen transfer process are rate-determining steps. The proposed mechanism can also be applied to the catalytic oxidation of sulfur mustard simulant.



中文翻译:

聚氧杂酸酯对神经毒剂VX模拟物的氧化解毒作用:实验和理论研究

VX是一种典型的神经毒剂,它的快速排毒作用取决于催化剂的发展以及对原子机理的理解。在此,我们报道Lindqvist型[Nb 6 O 19 ] 8-(Nb 6)可以有效地催化VX模拟物OSDEMP的解毒。在H 2 O 2存在下,OSDEMP可以在5分钟内完全转化为毒性最小的产品。各种实验证据:(1)DMNP(无S中心的有机磷酸酯)的转化率可忽略不计;(2)溶剂极性的影响;(3)18个O标记的实验证实了Nb 6对OSDEMP的解毒作用遵循氧化途径。进一步的实验和理论研究(例如光谱分析中,对照实验中,动力学研究,和DFT计算等)揭示的Nb(ƞ 1 -OOH)hexaniobate是主导活性种和Nb都形成(ƞ 1 -OOH)己酸铌的种类和氧的转移过程是决定速率的步骤。所提出的机理也可以应用于芥菜油模拟物的催化氧化。

更新日期:2021-01-05
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