采用共沉淀法制备了Co-Mn-Al层状双氢氧化物,并将其用于以硝基苯为目标污染物的催化臭氧降解反应中.结果表明,Co-Mn-Al层状双氢氧化物存在时,硝基苯的降解和矿化效率较单独臭氧氧化系统显著提高.采用加入羟基自由基捕获剂(叔丁醇)和电子顺磁共振检测(5,5-二甲基-1-吡咯啉-N-氧化物为捕获剂)的间接、直接方法,探讨了Co-Mn-Al层状双氢氧化物是否强化了羟基自由基的生成.结果表明,加入叔丁醇降低了硝基苯的降解效率；电子顺磁共振检出了更强的羟基自由基加成物生成信号.Co-Mn-Al层状双氢氧化物的存在促进了羟基自由基的生成.
The catalytic activity of layered double hydroxides containing Co,Mn,and Al for the ozonation of organic pollutants in water was investigated.The Co-Mn-Al layered double hydroxides were prepared by coprecipitation.Nitrobenzene was used as a model compound,and it was shown that the degradation and mineralization of nitrobenzene was increased by the presence of Co-Mn-Al layered double hydroxides as compared to ozonation alone.Both an indirect method of adding a scavenger (tert-butanol) of the hydroxyl radical chain reaction and direct electron spin resonance using 5,5-dimethyl-1-pyrroline-N-oxide as a spin trapping agent were used to investigate the generation of hydroxyl radicals in the ozonation by the Co-Mn-A1layered double hydroxides.The inhibiting effect of tert-butanol on the degradation of nitrobenzene and the detection of the stronger 5,5-dimethyl-1-pyrroline-N-oxide/hydroxyl radical adduct showed that the Co-Mn-Al layered double hydroxides catalyzed the generation of hydroxyl radicals.
参考文献
| [1] | Legube B;Leitner N K V .[J].Catalysis Today,1999,53:6l. |
| [2] | Kasprzyk-Hordem B;Ziólek M;Nawrocki J .[J].Applied Catalysis B:Environmental,2003,46:639. |
| [3] | Nawrocki J;Kasprzyk-Hordern B .[J].Applied Catalysis B:Environmental,2010,99:27. |
| [4] | 龙丽萍,赵建国,杨利娴,付名利,吴军良,黄碧纯,叶代启.常温下 MnO2/Al2O3催化剂催化臭氧氧化甲苯反应[J].催化学报,2011(06):904-916. |
| [5] | Chen Y H;Hsieh D C;Shang N C .[J].Journal of Hazardous Materials,2011,192:1017. |
| [6] | von Gunten U .[J].Water Research,2003,37:1443. |
| [7] | Dubey A;Rives V;Kannana S .[J].Journal of Molecular Catalysis A:Chemical,2002,181:151. |
| [8] | Goh K H;Lim T T;Dong Z L .[J].Water Research,2008,42:1343. |
| [9] | 刘诗咏,周其忠,金正能,蒋华江,姜玄珍.十二烷基磺酸根插层水滑石负载纳米钯催化的Suzuki偶联反应[J].催化学报,2010(05):557-561. |
| [10] | Staehelin J;Hoigné J .[J].Environmental Science and Technology,1982,16:676. |
| [11] | Hoigné J;BaderH .[J].Water Research,1983,17:173. |
| [12] | Faria P C C;Monteiro D C M;(O)rfao J J M;Pereira M F R .[J].Chemosphere,2009,74:818. |
| [13] | Alvarez, PM;Beltran, FJ;Pocostales, JP;Masa, FJ .Preparation and structural characterization of Co/Al2O3 catalysts for the ozonation of pyruvic acid[J].Applied Catalysis. B, Environmental,2007(3/4):322-330. |
| [14] | Lv A H;Hu C;Nie Y L;Qu J H .[J].Applied Catalysis B:Environmental,2010,100:62. |
| [15] | Kovanda F;Rojka T;Dobe(s)ová J;Machovi(o) V Bezdi(c)ka P Obalová L Jirátová K Grygar T .[J].Journal of Solid State Chemistry,2006,179:812. |
| [16] | Bader H;Hoigné J .[J].Water Research,1981,15:449. |
| [17] | Rakness K;Gordon G;Langlais B;Masschelein W Matsumoto N Richard Y Robson C M Somiya I .[J].Ozone Science and Engineering,1996,18:209. |
| [18] | Evans D G;Slade R C T .[J].Structure and Bonding,2006,119:1. |
| [19] | Manivannan R;Pandurangan A .[J].Applied Clay Science,2009,44:137. |
| [20] | Zhao Y;He J;Jiao Q Z;Evans D G Duan X Lu C H Wang Z G .[J].Chinese Journal of Inorganic Chemistry,2001,17:573. |
| [21] | Ervens B.;Gligorovski S.;Herrmann H. .Temperature-dependent rate constants for hydroxyl radical reactions with organic compounds in aqueous solutions[J].Physical chemistry chemical physics: PCCP,2003(9):1811-1824. |
| [22] | Han SK.;Utsumi H.;Ichikawa K. .Quantitative analysis for the enhancement of hydroxyl radical generation by phenols during ozonation of water[J].Water research: A journal of the international water association,1998(11):3261-3266. |
| [23] | Zhu BZ;Zhao HT;Kalyanaraman B;Frei B .Metal-independent production of hydroxyl radicals by halogenated quinones and hydrogen peroxide: an ESR spin trapping study.[J].Free Radical Biology & Medicine,2002(5):465-473. |
| [24] | Bosnjakovic A;Schlick S .[J].Journal of Physical Chemistry B,2006,110:10720. |
- 下载量()
- 访问量()
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%