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Degradation and fate of 2,4-dinitroanisole(DNAN)and its intermediates treated with Mg/Cu bimetal:Surface examination with XAS,DFT,and LDI-MS

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Journal of Environmental Sciences 2023年第7期129卷 161-173页

作者： Andrew Mai Emese Hadnagy Qiantao Shi Lotanna Ezeonu Jason P.Robbins Simon G.Podkolzin Agamemnon Koutsospyros christos christodoulatos Center for Environmental Systems Stevens Institute of TechnologyHobokenNJ 07030USA School of Engineering and Technology University of Washington TacomaTacomaWA 98402USA

A novel Mg-based bimetal reagent(Mg/Cu)was used as an enhanced reductive system to degrade insensitivemunition 2,4-dinitroanisole(DNAN),a contaminant found in energeticladenwaste.Degradation ofDNANwas significantly impacted by dissolved oxygen and studied in anoxic and oxic bimetal systems(i.e.,purging with N2,air,or O_(2) gas).Degradation occurred through sequential nitroreduction:first one nitro group was reduced(ortho or para)to form short-lived intermediates 2-amino-4-nitroanisole or 4-amino-2-nitroanisole(2-ANAN or 4-ANAN),and then subsequent reduction of the other nitro group formed 2,4-diaminoanisole(DAAN).The nitro-amino intermediates demonstrated regioselective reduction in the ortho position to 2-ANAN;Regioselectivity was also impacted by the anoxic/oxic environment.Under O_(2)-purging DNAN degradation rate was slightly enhanced,but most notably O_(2) significantly accelerated DAAN generation.DAAN also further degraded only in the oxygenated Mg/Cu system.Adsorption of DNAN byproducts to the reagent occurred regardless of anoxic/oxic condition,resulting in a partition of carbon mass between the adsorbed phase(27%-35%)and dissolved phase(59%-72%).Additional surface techniqueswere applied to investigate contaminant interaction with Cu.Density functional theory(DFT)calculations identified preferential adsorption structures for DNAN on Cu with binding through two O atoms of one or both nitro groups.X-ray absorption spectroscopy(XAS)measurements determined the oxidation state of catalyticmetal Cu and formation of a Cu-O-N bond during treatment.Laser desorption ionization mass spectrometry(LDI-MS)measurements also identified intermediate 2-ANAN adsorbed to the bimetal surface.

关键词： Insensitive munition Magnesium bimetal Reductive degradation Adsorption Surface analysis DFT DNAN Oxic

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Adsorption of Ca2+on single layer graphene oxide

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Journal of Environmental Sciences 2017年第7期29卷 8-14页

作者： Amalia Terracciano Jianfeng Zhang christos christodoulatos Fengchang Wu Xiaoguang Meng Center for Envronmental Systems Stevens Institute of TechnologyHobokenNJ 07030USA School of Environmental and Municipal Engineering Xi'an University of Architecture and TechnologyXi'an 710055China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China

Graphene oxide（GO） holds great promise for a broad array of applications in many fields,but also poses serious potential risks to human health and the environment.In this study,the adsorptive properties of GO toward Ca^（2＋） and Na＋were investigated using batch adsorption experiments,zeta potential measurements,and spectroscopic analysis.When pH increased from 4 to 9,Ca^（2＋）adsorption by GO and the zeta potential of GO increased significantly.Raman spectra suggest that Ca^（2＋）was strongly adsorbed on the GO via –COO Ca~＋ formation.On the other hand,Na＋was adsorbed into the electrical diffuse layer as an inert counterion to increase the diffuse layer zeta potential.While the GO suspension became unstable with increasing pH from 4 to 10 in the presence of Ca^（2＋）,it was more stable at higher pH in the NaC l solution.The findings of this research provide insights in the adsorption of Ca^（2＋）on GO and fundamental basis for prediction of its effect on the colloidal stability of GO in the environment.

关键词： Graphene oxide Calcium adsorption Raman spectra Colloidal stability

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Advanced Oxidation Process for DNAN Using UV/H2O2

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Engineering 2019年第5期5卷 849-854页

作者： Hailei Su christos christodoulatos Benjamin Smolinski Per Arienti Greg O’Connor Xiaoguang Meng Center for Environmental Systems Stevens Institute of TechnologyHobokenNJ 07030USA US Army RDECOM-ARDEC PicatinnyNJ 07806USA

2,4-Dinitroanisole(DNAN)is an important component of insensitive munitions that is anticipated to replace 2,4,6-trinitrotoluene(TNT)in munitions formulations.Photocatalyzed hydrogen peroxide(H2O2)oxidation experiments and chemical analyses were conducted to study the effect of initial pH and H2O2 dosage on the kinetics of DNAN decomposition and the reaction pathways.The results show that DNAN degradation followed zero-order kinetics when a 250 ppm DNAN solution was treated with ultraviolet(UV)light and 1500–4500 ppm H2O2 in an initial pH range of 4–7.However,when the H2O2 concentration was 750 ppm,DNAN degradation followed pseudo-first-order kinetics.The results indicate that DNAN can easily be oxidized by UV/H2O2 treatment.When the H2O2 dosage was 1500 ppm and the initial pH was 7,DNAN was reduced from 250 ppm to less than 1 ppm in 3 h.However,the total organic carbon(TOC)and total carbon(TC)concentrations were reduced slowly from 100 to less than 70 ppm carbon(C)in 3 h,and decreased to about 5 ppm after 9 h of treatment,suggesting the formation of other organic compounds.Those reaction intermediates were oxidized to carbon dioxide(CO2)at a slower rate than the oxidation of DNAN.CO2 was emitted from the solution because the solution pH decreased rapidly to about 3 during the UV/H2O2 oxidation.Most of the nitrogen in DNAN was converted to nitrate by UV/H2O2 oxidation after 9 h of treatment.The research results indicate that UV/H2O2 oxidation is a promising technique for the treatment of DNAN in wastewater.

关键词： 2,4-Dinitroanisole Advanced oxidation processes Wastewater treatment Photocatalysis

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