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Detoxification of mustard gas, nerve agents and simulants by peroxomolybdate in aqueous H2O2 solution: Reactive oxygen species and mechanisms

Sanping Zhao,Yong-bing Zhu,Hailing Xi,Mengwei Han,Daxue Li,Yang Li,Hongjie Zhao

Published 2020 in Journal of environmental chemical engineering

ABSTRACT

Abstract To overcome the insufficient understanding of the detoxification mechanisms of Chemical Warfare Agents (CWAs) and simulants by a molybdate-activated hydrogen peroxide solution (MoO42−-H2O2), detoxification performances toward CWAs and simulants were tested. The detoxification efficacy toward mustard gas (HD), nerve agent GD and VX by using MoO42−-H2O2 was higher than that by using H2O2 activated/modified by sodium hydroxide, ammonia, bicarbonate, and borates, but the vesicant mustard sulfone (HDO2) was only formed when using MoO42−-H2O2 to detoxify HD. Although Reactive Oxygen Species (ROS) such as singlet oxygen (1O2), superoxide anion (O2−), H2O2 and peroxide anion (OOH−) were detected by electron spin resonance (ESR) and chemiluminescence (CL) in the 0.1 M MoO42−-1.0 M H2O2 solution, 95Mo NMR indicated that Mo(O2)42− was the dominant oxidant for the oxidation of sulfide to sulfoxide and then to sulfone. Oxidation of HD by Mo(O2)42− occurred on the HD-drop/water interface through a direct oxygen transfer mechanism without the participation of H2O molecules, and further oxidation of HD to HDO2 was inevitable in an aqueous MoO42−-H2O2 solution. 18O tracer experiments confirmed that OOH−-based perhydrolysis dominated the detoxification reaction of nerve agents in an alkaline H2O2 solution. Considering the balance of oxidation/nucleophilic reactivity for a practical decontaminant, pH 10.5–11 range was recommended as the ideal for the MoO42−-H2O2 system to detoxify CWAs.

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