钙基复合氧化物对五氯酚生成二噁英的阻滞作用
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摘要
以市售的Ca O为阻滞剂,分别添加Mg O、Ce O2、Ba O、γ-Al2O3金属氧化物形成钙基复合氧化物,通过探究它们对前驱体五氯酚(PCP)生成PCDD/Fs反应的阻滞作用,讨论了Mg O、Ce O2、Ba O、γ-Al2O3金属氧化物对Ca O阻滞作用的影响.结果表明,在280℃下加热2 h,钙基复合氧化物对PCP生成PCDD/Fs的阻滞活性都很高.在PCDD/Fs的生成总量上,Ce O2、Ba O、γ-Al2O3金属氧化物对Ca O的阻滞效果起到促进作用;但在ITEQ方面,仅Ba O对Ca O的阻滞效果有促进作用.Ca O与Ba O钙基复合氧化物对PCP生成PCDD/Fs的阻滞效率达到99.98%,总毒性当量阻滞效率TSEI-TEQ达到99.62%.钙基复合氧化物可能的阻滞机理是Ca O、Mg O、Ce O2、Ba O、γ-Al2O3均具有一定的碱性,能与酚类前驱体发生中和反应,阻滞了Ullman反应的发生,进而减少了PCDD/Fs的生成.
Inhibition of calcium-based composite oxides on the formation of PCDD/Fs from PCP precursor was investigated in a laboratory-scale reactor at 280 ℃ for 2 h. The calcium-based composite oxides were prepared by mixing Ca O with Mg O,Ce O2,Ba O and γ-Al2O3,respectively.The results show that the total suppressing efficiency( TSE) of PCDD/Fs formation by these calcium-based composite oxides were all rather high. The addition of Ce O2,Ba O and γ-Al2O3 into Ca O reduced the total amount of produced PCDD/Fs. However,only Ba O increased the TSE in I-TEQ( TSEI-TEQ) of the newly formed PCDD/Fs. The TSE and TSEI-TEQof PCDD/Fs formation over Ca O and Ba O mixture were 99. 98% and 99. 62%,respectively. It was speculated that since Ca O,Mg O,Ce O2,Ba O and γ-Al2O3 are alkaline,they can react with the PCP precursor,to prevent the occurrence of Ullman reaction and the formation of PCDD/Fs.
Inhibition of calcium-based composite oxides on the formation of PCDD/Fs from PCP precursor was investigated in a laboratory-scale reactor at 280 ℃ for 2 h. The calcium-based composite oxides were prepared by mixing Ca O with Mg O,Ce O2,Ba O and γ-Al2O3,respectively.The results show that the total suppressing efficiency( TSE) of PCDD/Fs formation by these calcium-based composite oxides were all rather high. The addition of Ce O2,Ba O and γ-Al2O3 into Ca O reduced the total amount of produced PCDD/Fs. However,only Ba O increased the TSE in I-TEQ( TSEI-TEQ) of the newly formed PCDD/Fs. The TSE and TSEI-TEQof PCDD/Fs formation over Ca O and Ba O mixture were 99. 98% and 99. 62%,respectively. It was speculated that since Ca O,Mg O,Ce O2,Ba O and γ-Al2O3 are alkaline,they can react with the PCP precursor,to prevent the occurrence of Ullman reaction and the formation of PCDD/Fs.
引文
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[2]Jones K C,De Voogt P.Persistent organic pollutants(POPs):state of the science[J].Environmental Pollution,1999,100(1):209-221
[3]Atkinson R.Atmospheric chemistry of PCBs,PCDDs and PCDFs[J].Issues in environmental science and technology,1996,6:53-72
[4]Chen R J,Siao S H,Hsu C H,et al.TCDD promotes lung tumors via attenuation of apoptosis through activation of the Akt and ERK1/2signaling pathways[J].Plos One,2014,9(6):10
[5]Hoang T T,Traag W A,Murk A J,et al.Levels of polychlorinated dibenzo-p-dioxins,dibenzofurans(PCDD/Fs)and dioxin-like PCBs in free range eggs from Vietnam,including potential health risks[J].Chemosphere,2014,114:268-274
[6]Pelclova D,Prazny M,Skrha J,et al.2,3,7,8-TCDD exposure,endothelial dysfunction and impaired microvascular reactivity[J].Human&Experimental Toxicology,2007,26(9):705-713
[7]Ciftci O,Disli O M,Timurkaan N.Protective effects of protocatechuic acid on TCDD-induced oxidative and histopathological damage in the heart tissue of rats[J].Toxicology and Industrial Health,2013,29(9):806-811
[8]Wilhelm M,Wittsiepe J,Lemm F,et al.The Duisburg birth cohort study:Influence of the prenatal exposure to PCDD/Fs and dioxin-like PCBs on thyroid hormone status in newborns and neurodevelopment of infants until the age of 24 months[J].Mutation Research-Reviews in Mutation Research,2008,659(1-2):83-92
[9]Myrin E S,Persson P-E,Jansson S.The influence of food waste on dioxin formation during incineration of refuse-derived fuels[J].Fuel,2014,132:165-169
[10]Hu J C,Zheng M H,Liu W B,et al.Occupational exposure to polychlorinated dibenzo-p-dioxins and dibenzofurans,dioxin-like polychlorinated biphenyls,and polychlorinated naphthalenes in workplaces of secondary nonferrous metallurgical facilities in China[J].Environmental Science&Technology,2013,47(14):7773-7779
[11]Hu J,Zheng M,Liu W,et al.Characterization of polychlorinated dibenzo-p-dioxins and dibenzofurans,dioxin-like polychlorinated biphenyls,and polychlorinated naphthalenes in the environment surrounding secondary copper and aluminum metallurgical facilities in China[J].Environmental pollution(Barking,Essex:1987),2014,193:6-12
[12]Altarawneh M,Dlugogorski B Z,Kennedy E M,et al.Mechanisms for formation,chlorination,dechlorination and destruction of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)[J].Progress in Energy and Combustion Science,2009,35(3):245-274
[13]钱永,郑明辉,刘文彬,等.钙化合物对前生体生成二噁英类的阻滞作用[J].环境化学,2006,24(6):633-637
[14]Hajizadeh Y,Onwudili J A,Williams P T.Effects of gaseous NH3and SO2on the concentration profiles of PCDD/F in flyash under postcombustion zone conditions[J].Waste Management,2012,32(7):1378-1386
[15]Ma H,Liang P,Song X,et al.Synthesized inhibitors of PCDD/Fs when municipal solid wastes incinerated[J].Journal of Huazhong University of Science and Technology.Nature Science,2013,41(2):120-123
[16]Vollmuth S,Zajc A,Niessner R.Formation of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans during the photolysis of pentachlorophenol-containing water[J].Environmental science&technology,1994,28(6):1145-1149
[17]王贤,孙友敏,吴俊森.氯酚前驱物气相中形成二噁英物质(PCDD/Fs)的研究进展[J].山东师范大学学报(自然科学版),2012,1:126-129
[18]刘秡岩,郝吉明.氯酚为前生体生成二英类的研究进展[J].化学通报,2003,66(2):78-84
[19]Lu S,Chen T,Yan J,et al.Effects of calcium-based sorbents on PCDD/F formation from pentachlorophenol combustion process[J].Journal of hazardous materials,2007,147(1):663-671
[20]Qian Y,Zheng M,Liu W,et al.Influence of metal oxides on PCDD/Fs formation from pentachlorophenol[J].Chemosphere,2005,60(7):951-958
[21]Ingrosso G.Free radical chemistry and its concern with indoor air quality:an open problem[J].Microchemical journal,2002,73(1):221-236
[22]Brown S S,Stutz J.Nighttime radical observations and chemistry[J].Chemical Society Reviews,2012,41(19):6405-6447