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首页> 外文期刊>Environmental toxicology and chemistry >REDUCTIVE TRANSFORMATION OF HEXAHYDRO-1,3,5-TRINITRO-1,3,5-TRIAZINE, OCTAHYDRO-1,3,5,7-TETRANITRO-1,3,5,7-TETRAZOCINE, AND METHYLENEDINITRAMINE WITH ELEMENTAL IRON
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REDUCTIVE TRANSFORMATION OF HEXAHYDRO-1,3,5-TRINITRO-1,3,5-TRIAZINE, OCTAHYDRO-1,3,5,7-TETRANITRO-1,3,5,7-TETRAZOCINE, AND METHYLENEDINITRAMINE WITH ELEMENTAL IRON

机译：含铁的六亚甲基-1,3,5-三硝基-1,3,5-三嗪，八烷基-1,3,5,7-四硝基-1,3,5,7-四唑嗪和亚甲基间苯三胺的还原转化

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摘要

Reductive (pre)treatment with elemental iron is a potentially useful method for degrading nitramine explosives in water and soil. In the present study, we examined the kinetics, products, and mechanisms of hexahydro-1,3,5-trinitro-1,3,5-triazine(RDX) and octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX) degradation with elemental iron. Both RDX and HMX were transformed with iron to formaldehyde, NH_4~+, N_2O, and soluble products. The yields of formaldehyde were relatively constant (71% ± 5%), whereas the yields of NH_4~+ and N_2O varied, depending on the nitramine and the mechanism. The reactions most likely were controlled by a surface process rather than by external mass transfer. Methylenedinitramine (MDNA) was an intermediate of both RDX and HMX and was transformed quantitatively to formaldehyde with iron. However, product distributions and kinetic modeling results suggest that MDNA represented a minor reaction path and accounted for only 30% of the RDX reacted and 14% of the formaldehyde produced. Additional experiments showed that RDX reduction with elemental iron could be mediated by graphite and Fe~(2+) sorbed to magnetite, as demonstrated previously for nitroaromatics and nitrate esters. Methylenedinitramine was degraded primarily through reduction in the presence of elemental iron, because its hydrolysis was slow compared to its reactions with elemental iron and surface-bound Fe~(2+). Our results show that in a cast iron-water system, RDX may be transformed via multiple mechanisms involving different reaction paths and reaction sites.
机译：用元素铁进行还原（预处理）是降解水和土壤中硝胺炸药的潜在有用方法。在本研究中，我们研究了六氢-1,3,5-三硝基-1,3,5-三嗪（RDX）和八氢-1,3,5,7-四硝基-1的动力学，产物和机理，用元素铁降解3,5,7-四唑嗪（HMX）。 RDX和HMX均用铁转化为甲醛，NH_4〜+，N_2O和可溶性产物。甲醛的产率相对恒定（71％±5％），而NH_4〜+和N_2O的产率则取决于硝胺和机理。反应很可能是通过表面过程而不是外部传质控制的。亚甲二胺（MDNA）是RDX和HMX的中间体，并通过铁定量转化为甲醛。但是，产物分布和动力学建模结果表明，MDNA代表了次要的反应路径，仅占反应的RDX的30％和产生的甲醛的14％。额外的实验表明，元素铁还原RDX可以通过吸附到磁铁矿中的石墨和Fe〜（2+）来介导，如先前对硝基芳香族化合物和硝酸酯类的证明。亚甲基二乙胺主要通过在元素铁的存在下还原而降解，因为与与元素铁和表面结合的Fe〜（2+）的反应相比，其水解速度慢。我们的结果表明，在铸铁-水系统中，RDX可能通过涉及不同反应路径和反应部位的多种机理进行转化。

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