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首页> 外文期刊>Environmental Science & Technology >Exploring the Utility of Compound-Specific Isotope Analysis for Assessing Ferrous Iron-Mediated Reduction of RDX in the Subsurface
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Exploring the Utility of Compound-Specific Isotope Analysis for Assessing Ferrous Iron-Mediated Reduction of RDX in the Subsurface

机译：探讨复合特异性同位素分析的效用，用于评估地下铁晶铁介导的RDX

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摘要

Subsurface contamination with the explosive hexahydro-l,3,5-trinitro-l,3,5-triazine (RDX) at ordnance production and testing sites is a problem because of the persistence, mobility, and toxicity of RDX and the formation of toxic products under anoxic conditions. While the utility of compound-specific isotope analysis for inferring natural attenuation pathways from stable isotope ratios has been demonstrated, the stable isotope fractionation for RDX reduction by iron-bearing minerals remains unknown. Here, we evaluated N and C isotope fractionation of RDX during reduction by Fe(Ⅱ) associated with Fe minerals and natural sediments and applied N isotope ratios to the assessment of mineral-catalyzed RDX reduction in a contaminant plume and in sediment columns treated by in situ chemical reduction. Laboratory studies revealed that RDX was reduced to nitroso compounds without denitration and the concomitant ring cleavage. Fe(Ⅱ)/iron oxide mineral-catalyzed reactions exhibited N isotope enrichment factors, ε_N, between - 6.3±0.3‰ and -8.2±0.2‰, corresponding to an apparent ~(15)N kinetic isotope effect of 1.04-1.0S. The observed variations of the δ~(15)N of ～15‰ in RDX from groundwater samples suggested an extent of reductive transformation of 85% at an ammunition plant. Conversely, we observed masking of N isotope fractionation after RDX reduction in laboratory flow-through systems, which was presumably due to limited accessibility to reactive Fe(Ⅱ).
机译：随着爆炸性六羟基-L，3,5-三硝基-1，3,5-三嗪（RDX）的地下污染在军械生产和测试地点是一个问题，因为持续存在，流动性和RDX的毒性以及有毒的形成产品下的缺氧条件下。虽然已经证明了用于从稳定同位素比率推断自然衰减途径的复合特异性同位素分析的实用性，但通过铁矿物的RDX还原的稳定同位素分馏仍然未知。这里，我们在与Fe矿物质和天然沉积物相关的Fe（Ⅱ）减少期间评估了RDX的N和C同位素分馏，并施加了N同位素比，以评估矿物催化的RDX在污染物羽流和沉积物柱中的评估原位化学减少。实验室研究表明，在不脱硝的情况下，RDX降至亚硝基化合物和伴随的环裂解。 Fe（Ⅱ）/氧化铁矿物催化反应表现出N同位素富集因子，ε_n，6.3±0.3‰和-8.2±0.2‰，对应于1.04-1.0s的表观〜（15）n动力学同位素效应。从地下水样本的RDX中观察到δ〜（15）n的δ〜（15）n的变化表明弹药厂的还原转化程度为85％。相反，我们观察了在实验室流通系统的RDX降低后N同位素分馏的掩蔽，这可能是由于对反应性Fe的有限可接近（Ⅱ）。

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  • 来源
    《Environmental Science & Technology》 |2021年第10期|6752-6763|共12页
  • 作者

    Yiran Tong; Matthew J. Berens; Bridget A. Ulrich; Jakov Bolotin; Jennifer H. Strehlau; Thomas B. Hofstetter; William A. Arnold;

  • 作者单位

    Department of Civil Environmental and Geo-Engineering University of Minnesota Minneapolis Minnesota 55455-0116 United States;

    Department of Civil Environmental and Geo- Engineering University of Minnesota Minneapolis Minnesota 55455-0116 United States;

    Department of Environmental Chemistry Eawag Swiss Federal Institute of Aquatic Science and Technology CH-8600 Duebendorf Switzerland;

    Department of Environmental Chemistry Eawag Swiss Federal Institute of Aquatic Science and Technology CH-8600 Duebendorf Switzerland;

    Department of Civil Environmental and Geo- Engineering University of Minnesota Minneapolis Minnesota 55455-0116 United States;

    Department of Environmental Chemistry Eawag Swiss Federal Institute of Aquatic Science and Technology CH-8600 Duebendorf Switzerland;

    Department of Civil Environmental and Geo- Engineering University of Minnesota Minneapolis Minnesota 55455-0116 United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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