海水中原油光降解与TiO2光催化降解的比较研究Comparison Between Photolytic and Photocatalytic Degradation of Crude Oil by Nano-Titanium Dioxide in Seawater
崔玲君,张前前,李苓,张栋梅,安伟
摘要(Abstract):
本文采取与海洋环境相似的条件(海水介质、UV-A光照),设计长实验周期30d,对单纯光降解和TiO_2催化降解原油的行为进行了比较研究,着重考察研究了TiO_2催化剂用量、硬脂酸包裹与否等条件对原油降解率的影响,通过紫外光谱、总有机碳分析仪、柱层析、气相色谱质谱(GC-MS)法,分析了原油水溶性成分(Water Soluble Fractions:WSF)、溶解有机碳(DOC)、原油组成的改变。结果表明原油光催化降解率高于光降解,TiO_2催化剂用量对原油降解率及WSF的组成和浓度有显著影响,催化剂是否包裹则影响不大。TiO_2质量分数为12.5%时原油降解率为39.14%,水体中DOC含量最高达到89.60mg/L,多环芳烃的降解率高达82.97%。估算的胶质降解率与芳香烃组分的降解率呈现正相关,光催化使得正构烷烃组分含量升高。
关键词(KeyWords): 原油降解率;光降解;光催化降解;纳米TiO2;原油族组分;水溶性成分
基金项目(Foundation): 中海油“水下溢油行为模拟实验与深水区溢油应急技术研究”项目(CY-HB-12-ZC-121)资助~~
作者(Author): 崔玲君,张前前,李苓,张栋梅,安伟
DOI: 10.16441/j.cnki.hdxb.20150059
参考文献(References):
- [1]牟林,赵前.海洋溢油污染应急技术[M].北京:科学出版社,2011:225-253.Mu Lin,Zhao Qian.Emergency Response Technology for Marine Oil Spill Pollution[M].Beijing:Science Press,2011:225-253.
- [2]Hansen H P.Photochemical degradation of petroleum hydrocarbon surface films on seawater[J].Marine Chemistry,1975,3(3):183-195.
- [3]Shankar R,Shim W J,An J G,et al.A practical review on photooxidation of crude oil:Laboratory lamp setup and factors affecting it[J].Water Research,2015,68:304-315.
- [4]Payne J R,Phillips C R.Photochemistry of petroleum in water[J].Environmental Science and Technology,1985,19(7):569-579.
- [5]Ali L N,Mantoura R F C,Rowland S J.The dissolution and photodegradation of Kuwaiti crude oil in sea water.Part 1:Quantitative dissolution and analysis of the seawater-soluble fraction[J].Marine Environmental Research,1995,40(1):1-17.
- [6]Yang G P,et al.Photochemical degradation of crude oil in seawater[J].Chinese Journal of Oceanology and Limnology,2006,24(3):264-269.
- [7]Nair M,Luo Z,Heller A.Rates of photocatalytic oxidation of crude oil on salt water on buoyant,cenosphere-attached titanium dioxide[J].Industrial and Engineering Chemistry Research,1993,32(10):2318-2323.
- [8]Ziolli R L,Jardim W F.Photochemical transformations of watersoluble fraction(WSF)of crude oil in marine waters:A comparison between photolysis and accelerated degradation with TiO2using GC-MS and UVF[J].Journal of Photochemistry and Photobiology A:Chemistry,2003,155(1):243-252.
- [9]李秀芹,李子真,李春虎,等.Fe3+-TiO2/Shell光催化剂的制备及其对石油的光催化降解[J].石油学报(石油加工),2012,(6):1048-1052.Li Xiuqin,Li Zizhen,Li Chunhu,et al.Preparation of Fe3+xTiO2/Shell and photocatalytic degradation of oil pollutant suspension on the ocean[J].Acta Petrolei Sinica(Petroleum Processing Section),2012,(6):1048-1052.
- [10]Ray P Z,Tarr M A.Solar production of singlet oxygen from crude oil films on water[J].Journal of Photochemistry and Photobiology A:Chemistry,2014,286:22-28.
- [11]D’Auria M,Emanuele L,Racioppi R,et al.Photochemical degradation of crude oil:Comparison between direct irradiation,photocatalysis,and photocatalysis on zeolite[J].Journal of Hazardous Materials,2009,164(1):32-38.
- [12]Berry R J,Mueller M R.Photocatalytic decomposition of crude oil slicks using TiO2on a floating substrate[J].Microchemical Journal,1994,50(1):28-32.
- [13]Grzechulska J,Hamerski M,Morawski A W.Photocatalytic decomposition of oil in water[J].Water Research,2000,34(5):1638-1644.
- [14]于晓彩,杜倩,朱鹏飞,等.纳米TiO2光催化降解海洋石油污染[J].海洋环境科学,2011,(2):264-267.Yu Xiaocai,Du Qian,Zhu Pengfei,Yang li.Photo-catalytic degradation of petroleum in seawater by nano-titanium dioxide[J].Marine Environmental Science,2011,(2):264-267.
- [15]Jewell D M,Weber J H,Bunger J W,et al.Ion-exchange,coordination,and adsorption chromatographic separation of heavy-end petroleum distillates[J].Analytical Chemistry,1972,44(8):1391-1395.
- [16]Nicodem D E,Guedes C L B,Correa R J.Photochemistry of petroleum:I.Systematic study of a brazilian intermediate crude oil[J].Marine Chemistry,1998,63(1):93-104.
- [17]Maki H,Sasaki T,Harayama S.Photo-oxidation of biodegraded crude oil and toxicity of the photo-oxidized products[J].Chemosphere,2001,44(5):1145-1151.
- [18]Zhou Z,Liu Z,Guo L.Chemical evolution of Macondo crude oil during laboratory degradation as characterized by fluorescence EEMs and hydrocarbon composition[J].Marine Pollution Bulletin,2013,66(1):164-175.
- [19]Islam A,Cho Y,Yim U H,et al.The comparison of naturally weathered oil and artificially photo-degraded oil at the molecular level by a combination of SARA fractionation and FT-ICR MS[J].Journal of Hazardous Materials,2013,263:404-411.
- [20]Garrett R M,Pickering I J,Haith C E,et al.Photooxidation of crude oils[J].Environmental Science and Technology,1998,32(23):3719-3723.
- [21]King S M,Leaf P A,Olson A C,et al.Photolytic and photocatalytic degradation of surface oil from the Deepwater Horizon spill[J].Chemosphere,2014,95:415-422.
- [22]Ziolli R L,Jardim W F.Photocatalytic decomposition of seawater-soluble crude-oil fractions using high surface area colloid nanoparticles of TiO2[J].Journal of Photochemistry and Photobiology A:Chemistry,2002,147(3):205-212.
- [23]Pengerud B,Thingstad F,Tjessem K,et al.Photo-induced toxicity of North Sea crude oils toward bacterial activity[J].Marine Pollution Bulletin,1984,15(4):142-146.
- [24]EPA Method 3611B[S].Alumina Column Cleanup And Separation of Petroleum Wastes.
- [25]Wang Z,Fingas M,Li K.Fractionation of a light crude oil and identification and quantitation of aliphatic,aromatic,and biomarker compounds by GC-FID and GC-MS,part II[J].Journal of Chromatographic Science,1994,32(9):367-382.
- [26]粱文杰.石油化学[M].北京:石油大学出版社,1995:59-109.Liang Wenjie.Petroleum Chemistry[M].Beijing:China University of Petroleum Press,1995:59-109.
- [27]Brame J A,Hong S W,Lee J,et al.Photocatalytic pre-treatment with food-grade TiO2increases the bioavailability and bioremediation potential of weathered oil from the Deepwater Horizon oil spill in the Gulf of Mexico[J].Chemosphere,2013,90(8):2315-2319.
- [28]HeeáJang Y,HaáKim D.Efficient photocatalytic hybrid Ag/TiO2nanodot arrays integrated into nanopatterned block copolymer thin films[J].New Journal of Chemistry,2009,33(12):2431-2436.
- [29]张万忠,乔学亮,邱小林,等.纳米二氧化钛的光催化机理及其在有机废水处理中的应用[J].人工晶体学报,2006,35(5):1026-1031.Zhang Wanzhong,Qiao Xueliang,Qiu Xiaolin,et al.Photocatalytic mechanism of nano-titania and its application in the treatment of organic wastewater[J].Journal of Synthetic Crystals,2006,35(5):1026-1031.
- [30]何希杰,劳学苏.回归分析中临界相关系数的求值方法[J].河北工程技术高等专科学校学报,1993,2:12-19.He Xijie,Lao Xuesu.The evaluation method of critical correlation coefficient in regression analysis[J].Journal of Hebei Engineering and Technical College,1993,2:12-19.
- [31]Boukir A,Aries E,Guiliano M,et al.Subfractionation,characterization and photooxidation of crude oil resins[J].Chemosphere,2001,43(3):279-286.
- [32]Dutta T K,Harayama S.Fate of crude oil by the combination of photooxidation and biodegradation[J].Environmental Science and Technology,2000,34(8):1500-1505.
- [33]Wang Z,Fingas M F.Development of oil hydrocarbon fingerprinting and identification techniques[J].Marine Pollution Bulletin,2003,47(9):423-452.
文章评论(Comment):
|
||||||||||||||||||
|
||||||||||||||||||