Effects of oxidant and catalyst on the transformation products of rocket fuel 1,1-dimethylhydrazine in water and soil
Effects of oxidant and catalyst on the transformation products of rocket fuel 1,1-dimethylhydrazine in water and soil
复制标题
DOI：
10.1016/j.chemosphere.2019.04.141
复制
发表时间：
2019-08-01
期刊：
影响因子：
8.8
通讯作者：
Lebedev, Albert T.
中科院分区：
文献类型：
--
作者：
Kosyakov, Dmitry S.;Ul'yanovskii, Nikolay, V;Lebedev, Albert T.
现有的用于净化被剧毒火箭燃料偏二甲肼（UDMH）污染的废水和土壤的方法主要基于用各种氧化剂处理。到目前为止，对其有效性的评估是基于UDMH的残留含量，而没有考虑到形成大量潜在危险的含氮转化产物（Ws）的可能性。在这项研究中，使用最近开发的方法的基础上高分辨率轨道阱质谱，UDMH TP的综合表征形成的空气中的氧气和不同的氧化剂（芬顿的试剂，KMnO 4，HOCl，H2 O2的存在下的Cu 2+和[Fe（EDTA）]（-）催化剂）的作用通常用于解毒溢出网站进行。所鉴定的TP分子式的范围包括303种不同类别的化合物。其中，有一些主要产品以前没有在文献中描述。已经确定，所研究的氧化剂中没有一种能确保火箭燃料完全转化为安全化合物。基于过氧化氢的试剂，特别是目前在哈萨克斯坦使用的H2 O2 + Na [Fe（EDTA）]系统，产生的TP数量最多，其中许多毒性迄今尚未表征。在模型溶液中发现的大多数化合物是在质子号运载火箭坠毁地点的土壤提取物中检测到的，该地点曾进行过现场试剂处理。在连续的处理过程中，沿着可检测的UDMH TP数量的减少，它们的比例变化有利于胺。(C)2019爱思唯尔有限公司版权所有。
Existing methods for cleanup of wastewaters and soils polluted with the extremely toxic rocket fuel unsymmetrical dimethylhydrazine (UDMH) are mainly based on the treatment with various oxidative reagents. Until now, the assessment of their effectiveness was based on the residual content of UDMH and did not take into account the possibility of the formation of a large number of potentially dangerous nitrogen-containing transformation products (Ws). In this study, using the recently developed approach based on high-resolution Orbitrap mass spectrometry, the comprehensive characterization of UDMH TPs formed by the action of air oxygen and different oxidants (Fenton's reagent, KMnO4, HOCl, H2O2 in the presence of Cu2+ and [Fe (EDTA)](-) catalysts) typically used to detoxify spill sites was performed. The range of the identified molecular formulas of TPs comprised 303 compounds of various classes. Among them, there is a number of major products not previously described in the literature. It was established that none of the investigated oxidative reagents ensures complete conversion of rocket fuel to safe compounds. The hydrogen peroxide based reagents, particularly H2O2 + Na [Fe (EDTA)] system currently used in Kazakhstan, give the greatest number of TPs, for many of which a toxicity was not characterized so far. The majority of the compounds found in model solutions was detected in extracts of soil from the crash site of the Proton carrier rocket, which was subjected to the on-site reagent treatment. During successive treatments, along with the decrease in the number of detectable UDMH TPs, their ratios change in favor of amines. (C) 2019 Elsevier Ltd. All rights reserved.