水体中不同形态氮对阿昔洛韦光解的影响
Photodegradation of acyclovir in aquatic environment: Effect of different forms of nitrogen
-
摘要: 以350 W氙灯为太阳光模拟光源，探讨了水环境中不同形态氮（NO3-、NO2-和NH4+）对阿昔洛韦（ACV）光解的影响.结果表明，ACV在不同形态氮离子溶液中的光解符合一级动力学规律，NO3-和NO2-均促进ACV的光解，NH4+对ACV的光解基本无影响；在NO3-、NO2-存在下，加入异丙醇作为羟基自由基猝灭剂，显著抑制了ACV的降解，表明NO3-、NO2-在光照下产生了·OH参与ACV的氧化降解.同时模拟研究了水体处于不同pE值时，水中不同形态氮共存对ACV光解的复合影响.pE值增大，ACV的光解速率先增大后减小；当NO2-和NH4+共存时，对ACV的光解主要表现为NO2-的影响；当NO2-和NO3-共存时，两者对ACV的光解存在拮抗作用，说明其对ACV的光解不是简单的叠加.Abstract: Aqueous photolysis of acyclovir (ACV) using 350 W Xe lamp as simulated solar irradiation source was investigated in the presence of different forms (NO3-, NO2- and NH4+) of nitrogen. The results indicated that photodegradation of ACV in the solution of different forms of nitrogen ions followed pseudo-first-order kinetics. Nitrate and nitrite promoted photolysis of ACV. Ammonium ions had no influence on ACV photolysis. The photodegradation rate of ACV was significantly inhibited when an appropriate amount of isopropanol was added in the presence of nitrate or nitrite. This phenomenon manifested that hydroxyl radical was produced during the experiment and enhanced the degradation rate of ACV. Photodegradation of ACV was also investigated under diverse pE values. The photodegradation rate of ACV increased first then decreased with increasing pE values. Nitrite played a key role in the photolysis of ACV when it coexisted with ammonium. The antagonistic effect existed on the photolysis of ACV when nitrate coexisted with nitrite, which indicates it's effect on the photodegradation of ACV isn't simply additive.
-
Key words:
- acyclovir /
- photodegradation /
- inorganic nitrogen /
- pE values /
- hydroxyl radical
-
-
[1] DAUGHTON C G, TERNES T A. Pharmaceuticals and personal care products in the environment:Agents of subtle change?[J]. Environmental Health Perspectives, 1999, 107:907. [2] KOSMA C I, LAMBROPOULOU D A, ALBANIS T A. Investigation of PPCPs in wastewater treatment plants in Greece:Occurrence, removal and environmental risk assessment[J]. Science of the Total Environment, 2014, 466:421-438. [3] PECK A M. Analytical methods for the determination of persistent ingredients of personal care products in environmental matrices[J]. Analytical and Bioanalytical Chemistry, 2006, 386(4):907-939. [4] WESTERHOFF P, YOON Y, SNYDER S, et al. Fate of endocrine-disruptor, pharmaceutical, and personal care product chemicals during simulated drinking water treatment processes[J]. Environmental Science & Technology, 2005, 39(17):6649-6663. [5] JOLANTA DEBSKA A K J N. Fate and analysis of pharmaceutical residues in the aquatic environment[J]. Critical Reviews in Analytical Chemistry, 2004, 34(1):51-67. [6] KOLPIN D W, FURLONG E T, MEYER M T, et al. Pharmaceuticals, hormones, and other organic wastewater contaminants in US streams, 1999-2000:A national reconnaissance[J]. Environmental Science & Technology, 2002, 36(6):1202-1211. [7] PAROLINI M, PEDRIALI A, BINELLI A. Application of a biomarker response index for ranking the toxicity of five pharmaceutical and personal care products (PPCPs) to the Bivalve Dreissena polymorpha[J]. Archives of Environmental Contamination & Toxicology, 2013, 64(3):439-447. [8] DAUGHTON C G, JONES-LEPP T L. Pharmaceuticals and personal care products in the environment:Scientific and regulatory issues[M]. Washington, DC:American Chemical Society, 2001:2-38. [9] BRAIN R A, RAMIREZ A J, FULTON B A, et al. Herbicidal effects of sulfamethoxazole in Lemna gibba:Using p-aminobenzoic acid as a biomarker of effect[J]. Environmental Science & Technology, 2008, 42(23):8965-8970. [10] BROWN S D, WHITE C A, BARTLETT M G. Hydrophilic interaction liquid chromatography/electrospray mass spectrometry determination of acyclovir in pregnant rat plasma and tissues[J]. Rapid Communications in Mass Spectrometry, 2002, 16(19):1871-1876. [11] 安继斌. 水体中典型有机污染物的光催化降解动力学及降解机理研究[D]. 兰州:兰州理工大学硕士学位论文, 2011. AN J B. Photocatalytic degradation kinetics and mechanism of model organic pollutants in water environment[D]. Lanzhou:Lanzhou University of Technology,Master Thsis, 2011(in Chinese). [12] PENG X, ZHANG K, TANG C, et al. Distribution pattern, behavior, and fate of antibacterials in urban aquatic environments in South China.[J]. Journal of Environmental Monitoring, 2011, 13(2):446-454. [13] Klaus K. Antibiotics in the aquatic environment-a review-part Ⅱ[J]. Chemosphere, 2009, 75(4):417-434. [14] AN T, LI G, SONG W, et al. Photocatalytic degradation and mineralization mechanism and toxicity assessment of antivirus drug acyclovir:Experimental and theoretical studies[J]. Applied Catalysis B Environmental, 2015, 164:279-287. [15] PRASSE C, WAGNER M, SCHULZ R, et al. Oxidation of the antiviral drug acyclovir and its biodegradation product carboxy-acyclovir with ozone:Kinetics and identification of oxidation products[J]. Environmental Science & Technology, 2012, 46(4):2169-2178. [16] CARSTEN P, MANFRED W, RALF S, et al. Biotransformation of the antiviral drugs acyclovir and penciclovir in activated sludge treatment[J]. Environmental Science & Technology, 2011, 45(7):2761-2769. [17] ROBINSON P F, LIU Q T, RIDDLE A M, et al. Modeling the impact of direct phototransformation on predicted environmental concentrations (PECs) of propranolol hydrochloride in UK and US rivers[J]. Chemosphere, 2007, 66(4):757-766. [18] ZHANG N, LIU G, LIU H, et al. Diclofenac photodegradation under simulated sunlight:Effect of different forms of nitrogen and kinetics[J]. Journal of Hazardous Materials, 2011, 192(1):411-418. [19] 葛林科. 水中溶解性物质对氯霉素类和氟喹诺酮类抗生素光降解的影响[D]. 大连:大连理工大学博士学位论文, 2009. GE L K. Effects of aqueous dissolved matter on photodegradation of phenicol and fluoroquinolone antibiotics[D]. Dalian:Dalian University of Technology,Doctor Thsis, 2009(in Chinese). [20] LIU G, LIU H, ZHANG N, et al. Photodegradation of salicylic acid in aquatic environment:Effect of different forms of nitrogen[J]. Science of the Total Environment, 2012, 435:573-577. [21] 马杜娟. 水环境中萘普生光化学降解行为研究[D]. 广州:广东工业大学硕士学位论文, 2013. MA D J. The study of photolytic behavior of naproxen in aqueous environment[D]. Guangzhou:Guangdong University of Technology,Master Thsis, 2013(in Chinese). [22] 李超, 谢国红, 刘国光, 等. 不同形态氮转化对啶虫脒在水溶液中光解的影响[J]. 环境科学学报, 2009, 29(9):1918-1922. LI C, XIE G H, LIU G G, et al. The role of different forms of inorganic nitrogen in the photolysis of acetamiprid[J]. Journal of environmental science, 2009, 29(9):1918-1922(in Chinese).
[23] ZAFIRIOU O C, TRUE M B. Nitrite photolysis in seawater by sunlight[J]. Marine Chemistry, 1979, 8(1):9-32. [24] NATO. Advanced Study Institute on Oxygen Radicals in Biological Systems:Recent Progress and New Study Methods, Quintanilha A T. Reactive Oxygen Species in Chemistry, Biology, and Medicine[M]. Springer US, 2013. [25] MACK J, BOLTON J R. Photochemistry of nitrite and nitrate in aqueous solution:A review[J]. Journal of Photochemistry & Photobiology A Chemistry, 1999, 128(1):1-13. [26] 张敏利, 刘国光, 张楠,等. 不同形态氮对水中4,4'-二溴联苯光解的影响[J]. 环境化学, 2015, 30(3):604-608. ZHANG M L, LIU G G, ZHANG N,et al. The effect of different nitrogen forms on the photodegradation of 4, 4'-bromine biphenyl 2 in Water[J]. Environmental Chemistry, 2015, 30(3):604-608(in Chinese).
[27] 陈平, 刘国光, 吕文英,等. 水环境中不同形态氮对甲芬那酸光降解影响机制的研究[J].环境科学学报, 2015, 35(10):3151-3156. CHEN P, LIU G G, LYU W Y,et al. Photodegradation of mefenamic acid in aquatic environment:effect of different forms of nitrogen[J]. Journal of Environmental Science, 2015, 35(10):3151-3156(in Chinese).
[28] BUXTON G V, GREENSTOCK C L, HELMAN W P, et al. Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (·OH/·O-in Aqueous Solution[J]. Journal of Physical & Chemical Reference Data, 1988, 17(2):513-886. -
点击查看大图
计量
- 文章访问数: 1223
- HTML全文浏览数: 1160
- PDF下载数: 509
- 施引文献: 0
下载:
