Monitoring of the total carbon and nitrogen balance during the mineralization of nitrogen containing compounds by heat activated persulfate

被引:8
作者
Koester, Daniel [1 ]
Jochmann, Maik A. [1 ,2 ]
Lutze, Holger, V [1 ,2 ,3 ]
Schmidt, Torsten C. [1 ,2 ,3 ]
机构
[1] Univ Duisburg Essen, Instrumental Analyt Chem, Univ Str 5, D-45141 Essen, Germany
[2] Univ Duisburg Essen, Ctr Water & Environm Res ZWU, Univ Str 5, D-45141 Essen, Germany
[3] IWW Water Ctr, Moritzstr 26, D-45476 Mulheim, Germany
关键词
Peroxydisulfate; Mineralization products; Mass balance; Nitrogen species; Ion chromatography; Total nitrogen bound; SULFATE RADICALS; WATER-TREATMENT; RATE CONSTANTS; AMMONIUM-IONS; WASTE-WATER; OXIDATION; KINETICS; DEGRADATION; TEMPERATURE; CHEMISTRY;
D O I
10.1016/j.cej.2019.02.115
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Peroxydisulfate (S2O82-) is widely applied in environmental remediation and water treatment as an agent for the unselective oxidation of organic contaminants. S2O82- itself is a strong oxidation agent but activation by heat, UV radiation, or metal catalysts forms sulfate radicals (SO4 center dot-), which offer a higher oxidation potential and faster reaction kinetics. The mechanism of degradation for many organic contaminants by sulfate radicals is well studied, but the final mineralization products are not commonly evaluated. Nitrogen containing compounds are known to produce different mineralization products depending on their structure and the reaction conditions. For the identification of the main mineralization products, two approaches for the determination of nitrogen mass balances were evaluated. The first approach was based on a combination of total organic carbon (TOC), and total nitrogen bound (TNb). The second approach used a combination of TOC and ion chromatography (IC). The evaluation based on the TOC and TNb by high temperature combustion was found to be significantly biased as measured ammonium concentrations were underestimated by the TNb measurements in the presence of peroxydisulfate. With the TOC/TNb method, 83.2 +/- 1.1% of the initial nitrogen could be recovered after the oxidation. The TOC/IC based approach led to an overall recovery of 91.1 +/- 1.4%, where NO3- and NH4+ were identified as the main products. Based on the fraction of ammonium provided by the IC measurements, the TOC/TNb based results could be corrected for the underestimation of ammonium which led to a recovery of 95.9 +/- 3.1%. The presented methods are applicable for the determination of nitrogen mass balances in lab-scale studies, as well as for the monitoring of mineralization products in field applications.
引用
收藏
页码:160 / 168
页数:9
相关论文
共 36 条
[1]   Simultaneous determination of TOC and TNb in surface and wastewater by optimised high temperature catalytic combustion [J].
Ammann, AA ;
Rüttimann, TB ;
Bürgi, F .
WATER RESEARCH, 2000, 34 (14) :3573-3579
[2]   Radical generation by the interaction of transition metals with common oxidants [J].
Anipsitakis, GP ;
Dionysiou, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (13) :3705-3712
[3]  
[Anonymous], 2008, DIN 32645:2008-11.
[4]  
[Anonymous], 1997, EN1484
[5]   Sodium peroxydisulfate is a stable and cheap substitute for ammonium peroxydisulfate (persulfate) in polyacrylamide gel electrophoresis [J].
Behrman, EJ ;
Dean, DH .
JOURNAL OF CHROMATOGRAPHY B, 1999, 723 (1-2) :325-326
[6]   Total dissolved nitrogen analysis: comparisons between the persulfate, UV and high temperature oxidation methods [J].
Bronk, DA ;
Lomas, MW ;
Glibert, PM ;
Schukert, KJ ;
Sanderson, MP .
MARINE CHEMISTRY, 2000, 69 (1-2) :163-178
[7]   RATE CONSTANTS FOR HYDROGEN ABSTRACTION REACTIONS OF THE SULFATE RADICAL, SO4- - ALCOHOLS [J].
CLIFTON, CL ;
HUIE, RE .
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS, 1989, 21 (08) :677-687
[8]   DETERMINATION OF TOTAL NITROGEN IN AQUEOUS SAMPLES USING PERSULFATE DIGESTION [J].
DELIA, CF ;
STEUDLER, PA ;
CORWIN, N .
LIMNOLOGY AND OCEANOGRAPHY, 1977, 22 (04) :760-764
[9]   Mineralization of aniline using hydroxyl/sulfate radical-based technology in a waterfall reactor [J].
Duran, A. ;
Monteagudo, J. M. ;
San Martin, I. ;
Amunategui, F. J. ;
Patterson, D. A. .
CHEMOSPHERE, 2017, 186 :177-184
[10]   SIMULTANEOUS DETERMINATION OF TOTAL NITROGEN AND TOTAL PHOSPHORUS IN WATER USING PEROXODISULFATE OXIDATION [J].
EBINA, J ;
TSUTSUI, T ;
SHIRAI, T .
WATER RESEARCH, 1983, 17 (12) :1721-1726