Kitcher E, Braida W, Koutsospyros A, Pavlov J, Su T-L
Center for Environmental Systems, Stevens Institute of Technology, Hoboken, NJ, 07030, USA.
University of New Haven, 300 Boston Post Road, West Haven, CT, 06516, USA.
Environ Sci Pollut Res Int. 2017 Jan;24(3):2744-2753. doi: 10.1007/s11356-016-8053-7. Epub 2016 Nov 11.
It has been shown previously that, under acidic conditions, 3-nitro-1,2,4-triazol-5-one (NTO) and 2,4-dinitroanisole (DNAN) degrade in the presence of iron/copper bimetal particles; the reactions can be modeled by pseudo-first-order kinetics. This study investigates the reaction mechanisms of the degradation processes under different conditions. Batch studies were conducted using laboratory-prepared solutions and an industrial insensitive munition-laden (IMX) wastewater. The influence of parameters such as initial pH of the solution, copper/iron (Fe-Cu) contact, and solid/liquid ratio were systematically investigated to assess their impact on the reaction kinetics. These parameters were subsequently incorporated into pseudo-first-order decomposition models for NTO and DNAN. The activation energies for the degradation reactions were 27.40 and 30.57 kJ mol, respectively. Degradation intermediates and products were identified. A nitro-to-amino pathway, which ultimately may lead to partial mineralization, is postulated. The amino intermediate, aminonitroanisole, was detected during DNAN degradation, but for NTO, aminotiazolone is suggested. Additionally, urea was identified as a degradation product of NTO.
先前已表明,在酸性条件下,3-硝基-1,2,4-三唑-5-酮(NTO)和2,4-二硝基苯甲醚(DNAN)在铁/铜双金属颗粒存在下会降解;这些反应可用准一级动力学进行模拟。本研究考察了不同条件下降解过程的反应机理。使用实验室配制的溶液和含工业钝感弹药(IMX)的废水进行了批次研究。系统研究了溶液初始pH值、铜/铁(Fe-Cu)接触情况和固液比等参数的影响,以评估它们对反应动力学的影响。随后将这些参数纳入NTO和DNAN的准一级分解模型。降解反应的活化能分别为27.40和30.57 kJ/mol。鉴定出了降解中间体和产物。推测了一条硝基到氨基的途径,该途径最终可能导致部分矿化。在DNAN降解过程中检测到了氨基中间体氨基硝基苯甲醚,但对于NTO,推测为氨基噻唑酮。此外,尿素被鉴定为NTO的降解产物。