亚铁离子/四聚磷酸活化分子氧降解氯霉素
Dioxygen activation by Fe(Ⅱ)-Tetrapolyphosphate(TPP) complex for the degradation of chloramphenicol
-
摘要: 本文研究了亚铁离子(Fe2+)/四聚磷酸(TPP)/空气(Air)体系降解有机污染物氯霉素(CAP)的能力.研究发现,在氩气(Ar)氛围中和用乙二胺四乙酸(EDTA)代替TPP配体后均不能有效降解CAP,只有在Fe2+、TPP、Air共存时才能够有效降解CAP.结合活性氧测试及自由基捕获实验,表明Fe2+/TPP配合物活化分子氧是该体系降解有机污染物的关键,反应过程中生成超氧阴离子自由基(·O2-)和羟基自由基(·OH),其中·OH在CAP降解过程中起主要作用.随着反应的进行,体系中的Fe2+逐渐转化为Fe3+,失去活化分子氧的能力,也不再能够降解CAP.上述降解过程中脱氯量为10%,总有机碳去除率为20%,综合气质联用仪(GC-MS)以及液质联用仪(LC-MS)测得的中间体物种,推测了CAP降解的可能机理.进一步研究表明,在中性及弱碱性条件下该体系对CAP具有较强的降解能力,为其用于CAP污染物的处理提供了可能.Abstract: The ability of Fe2+/TPP/Air system to degrade chloramphenicol (CAP) was evaluated in this study. For comparison, controlled experiments were conducted by replacing the air and TPP with Ar and EDTA respectively. It was found that the CAP could only be effectively degraded in the presence of Fe2+, TPP and Air. The activation of molecular oxygen by the complexes of TPP and Fe2+ played a dominant role in the degradation of organic pollutants. Two free radicals, ·O2- and ·OH, were generated in this system, whilst the ·OH radical played a dominant role in pollutant degradation. CAP was degraded until Fe2+ in the system was completely oxidized to Fe3+. TOC experimental results showed that the mineralization rate of CAP in this system was 20%. The dechlorination rate was 10%. Based on the intermediate species measured by the GC-MS and LC-MS, the possible degradation mechanism of CAP was proposed. The Fe2+/TPP/Air system worked well for the degradation of CAP under the neutral and weakly alkaline conditions, and would be an alternative technology for CAP removal.
-
Key words:
- chloramphenicol /
- Fe2+ ions /
- tetrapolyphosphate /
- dioxygen
-
[1] RABIET M, TOGOLA A, BRISSAUD F, et al. Consequences of treated water recycling as regards pharmaceuticals and drugs in surface and ground waters of a medium-sized mediterranean catchment[J]. Environmental Science & Technology, 2006, 40(17):5282-5288. [2] 刘奇, 魏东斌, 陈振斌,等. 医药品和个人护理用品(PPCPs)类污染物氯化转化行为研究进展[J]. 环境化学, 2012, 31(3):278-286. LIU Q, WEI D, CHEN Z, et al. A review on transformation behaviors of PPCPs in chlorination process[J]. Environmental Chemistry, 2012, 31(3):278-286(in Chinese).
[3] KARTHIK R, KUMAR J, CHEN S, et al. A Study of electrocatalytic and photocatalytic activity of cerium molybdate nanocubes decorated graphene oxide for the sensing and degradation of antibiotic drug chloramphenicol[J]. ACS Applied Materials & Interfaces, 2017, 9:6547-6559. [4] 李春颖, 赖克强, 张源园,等. 表面增强拉曼光谱检测鱼肉中禁用和限用药物研究[J]. 化学学报, 2013, 71(2):221-226. LI C, LAI K, ZHANG Y, et al. Use of surface-enhanced raman spectroscopy for the test of residuals of prohibited and restricted drugs in fish muscle[J]. Acta Chimica Sinica, 2013, 71(2):221-226(in Chinese).
[5] ZHANG Q, ZHANG Y, LI D. Cometabolic degradation of chloramphenicol via a meta-cleavage pathway in a microbial fuel cell and its microbial community[J]. Bioresource Technology, 2017, 229:104-110. [6] NIE M, YAN C, LI M, et al. Degradation of chloramphenicol by persulfate activated by Fe2+, and zerovalent iron[J]. Chemical Engineering Journal, 2015, 279:507-515. [7] BADAWY M I, WAHAAB R A, ELKALLINY A S. Fenton-biological treatment processes for the removal of some pharmaceuticals from industrial wastewater[J]. Journal of Hazardous Materials, 2009, 167(1-3):567-574. [8] LOFRANO G, LIBRALATO G, ADINOLFI R, et al. Photocatalytic degradation of the antibiotic chloramphenicol and effluent toxicity effects[J]. Ecotoxicology & Environmental Safety, 2016, 123:65-71. [9] JOSS A, ZABDZYNSKI S, GOBEL A, et al. Biological degradation of pharmaceuticals in municipal wastewater treatment:Proposing a classification scheme[J]. Water Research, 2006, 40(8):1686-1696. [10] FAN Y, WANG B, YUAN S H, et al. Adsorptive removal of chloramphenicol from wastewater by NaOH modified bamboo charcoal[J]. Bioresource Technology, 2010, 101(19):7661-7664. [11] ARSLAN-ALATON I, GURSES F. Photo-Fenton-like and photo-Fenton-like oxidation of procaine Penicillin G formulation effluent[J]. Journal of Photochemistry & Photobiology A Chemistry, 2004, 165(1):165-175. [12] TROVO A G, NOGUEIRA R F, AGUERA A, et al. Photodegradation of sulfamethoxazole in various aqueous media:Persistence, toxicity and photoproducts assessment[J]. Chemosphere 2009, 77(10):1292-1298. [13] HUG S J, LEUPIN O. Iron-catalyzed oxidation of arsenic(Ⅲ) by oxygen and by hydrogen peroxide:pH-dependent formation of oxidants in the Fenton reaction[J]. Environmental Science & Technology. 2003, 37(12):2734-2742. [14] ARIKAN O A. Degradation and metabolization of chlortetracycline during the anaerobic digestion of manure from medicated calves[J]. Journal of Hazardous Materials, 2008, 158(2/3):485-490. [15] MENDEZ-DIAZ J D, PRADOS-JOYA G, RIVERA-UTRILLA J, et al. Kinetic study of the adsorption of nitroimidazole antibiotics on activated carbons in aqueous phase[J]. Journal of Colloid & Interface Science, 2010, 345(2):481-490. [16] BIAGLOW J E, KACHUR A V. The generation of hydroxyl radicals in the reaction of molecular oxygen with polyphosphate complexes of ferrous ion[J]. Radiation Research, 1997, 148(2):181-187. [17] WELCH K D, DAVIS T Z, AUST S D. Iron autoxidation and free radical generation:Effects of buffers, ligands, and chelators[J]. Archives of Biochemistry & Biophysics, 2002, 397(2):360-369. [18] KEENAN C R, SEDLAK D L. Ligand-enhanced reactive oxidant generation by nanoparticulate zero-valent iron and oxygen[J]. Environmental Science & Technology, 2011, 42(18):6936-6941. [19] WANG L, WANG F, LI P, et al. Ferrous-tetrapolyphosphate complex induced dioxygen activation for toxic organic pollutants degradation[J]. Separation & Purification Technology, 2013, 120:148-155. [20] WANG L, CAO M, AI Z, et al. Dramatically enhanced aerobic atrazine degradation with Fe@Fe2O3 core-shell nanowires by tetrapolyphosphate[J]. Environmental Science & Technology, 2014, 48(6):3354-3362. [21] WANG L, CAO M, AI Z, et al. Design of a highly efficient and wide pH electro-Fenton oxidation system with molecular oxygen activated by ferrous-tetrapolyphosphate complex[J]. Environmental Science & Technology, 2015, 49(5):3032-3039. [22] DENG J, FENG S F, ZHANG K, et al. Heterogeneous activation of peroxymonosulfate using ordered mesoporous Co3O4, for the degradation of chloramphenicol at neutral pH[J]. Chemical Engineering Journal, 2016, 308:505-515. [23] JR A E H, SMART J A, AMIS E S. Simultaneous spectrophotometric determination of Iron(Ⅱ) and total iron with 1,10-phenanthroline[J]. Analytical Chemistry, 1955, 27(1):26-29. [24] LIU W, AI Z H, CAO M H, et al. Ferrous ions promoted aerobic simazine degradation with Fe@Fe2O3, core-shell nanowires[J]. Applied Catalysis B Environmental, 2014, 150-151:1-11. [25] SANCHEZ I, STUBER F, FONT J, et al. Elimination of phenol and aromatic compounds by zero valent iron and EDTA at low temperature and atmospheric pressure[J]. Chemosphere, 2007, 68(2):338-344.
计量
- 文章访问数: 1097
- HTML全文浏览数: 1030
- PDF下载数: 344
- 施引文献: 0