二价铁催化过氧化氢-过硫酸钠再生活性炭可行性研究
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摘要
利用二价铁(Fe~(2+))催化过氧化氢(H_2O_2)-过硫酸钠(Na_2S_2O_8)双氧化体系(ICHP)对被三氯乙烯(TCE)吸附饱和的20~40目粒状活性炭(AC)进行再生研究.同时,结合扫描电子显微镜(SEM)、能量散射光谱仪(EDS)、X射线光电子能谱仪(XPS)及氮气吸附-解吸技术等手段对再生前后的AC进行表征,进一步探讨影响再生效率的原因.结果表明,AC对TCE的吸附符合准一级动力学模型,等温吸附符合Freundlich模型.在TCE∶Fe~(2+)∶H_2O_2∶S_2O_2-8=1∶9.20∶59.79∶77.52(物质的量比)的条件下,AC再生效率约为50%.研究表明,AC的炭损失、比表面积、孔隙体积及孔隙面积的减小,是再生AC吸附能力低于原状AC的主要原因.利用ICHP再生的AC可以实现对TCE的有效吸附并达到AC重复使用的目的,具有很好的实用价值.
A binary catalytic system,ferrous ion( Fe~(2+))-catalyzed hydrogen peroxide( H_2 O_2) coupled with sodium persulfate( Na_2 S_2 O_8)( ICHP),was investigated for the regeneration of 20 ~ 40 mesh activated carbon( AC) adsorbed by trichloroethylene( TCE). The Scanning Electron Microscope( SEM),Energy Dispersive Spectrometer( EDS),X-ray Photoelectron Spectroscopy( XPS),Nitrogen Adsorption-Desorption Techniques were used to further investigate the influence of regeneration efficiency. The results indicated that the adsorption of TCE on AC followed pseudo first-order kinetic model and Freundlich model. The regeneration efficiency of AC was 50% when TCE ∶ Fe~(2+)∶ H_2 O_2∶ S_2 O_2-8= 1∶ 9.20∶ 59.79∶ 77.52 in molar ratio was used. The carbon loss,the decrease in surface area,pore volume,and aperture area were the main factors which inhibited the efficiency of the regenerated AC. The results of this study indicate that the regeneration of AC by ICHP achieves high TCE adsorption efficiency,and therefore achieves the recycling of AC,which provides the good practical value.
A binary catalytic system,ferrous ion( Fe~(2+))-catalyzed hydrogen peroxide( H_2 O_2) coupled with sodium persulfate( Na_2 S_2 O_8)( ICHP),was investigated for the regeneration of 20 ~ 40 mesh activated carbon( AC) adsorbed by trichloroethylene( TCE). The Scanning Electron Microscope( SEM),Energy Dispersive Spectrometer( EDS),X-ray Photoelectron Spectroscopy( XPS),Nitrogen Adsorption-Desorption Techniques were used to further investigate the influence of regeneration efficiency. The results indicated that the adsorption of TCE on AC followed pseudo first-order kinetic model and Freundlich model. The regeneration efficiency of AC was 50% when TCE ∶ Fe~(2+)∶ H_2 O_2∶ S_2 O_2-8= 1∶ 9.20∶ 59.79∶ 77.52 in molar ratio was used. The carbon loss,the decrease in surface area,pore volume,and aperture area were the main factors which inhibited the efficiency of the regenerated AC. The results of this study indicate that the regeneration of AC by ICHP achieves high TCE adsorption efficiency,and therefore achieves the recycling of AC,which provides the good practical value.
引文
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Narbaitz R M,Cen J.1997.Alternative methods for determining the percentage regeneration of activated carbon[J].Water Research,31(31):2532-2542
Quinlivan P A,Li L,Knappe D R.2005.Effects of activated carbon characteristics on the simultaneous adsorption of aqueous organic micropollutants and natural organic matter[J].Water Research,39(8):1663-1673
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王宝庆,陈亚雄,宁平.2000.活性炭水处理技术应用[J].环境科学导刊,19(3):46-49
王福禄.2011.Fenton试剂再生活性炭的试验研究[J].工业用水与废水,42(3):48-51
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Yamashita T,Hayes P.2008.Analysis of XPS spectra of Fe2+,and Fe3+,ions in oxide materials[J].Applied Surface Science,254(8):2441-2449
Yan N,Liu F,Xue Q,et al.2015.Degradation of trichloroethene by siderite-catalyzed hydrogen peroxide and persulfate:Investigation of reaction mechanisms and degradation products[J].Chemical Engineering Journal,274:61-68
曾雪玲,唐晓东,卢涛.2008.活性炭再生技术的研究进展[J].四川化工,11(4):11-15
周琴,沈健,黄敏.2013.活性炭的制备及再生研究进展[J].化学与生物工程,30(12):10-13
顾广隽,孙香潭.1985.活性炭吸附焦化污水中某些无机离子的行为[J].环境化学,4(6):58-62
韩庭苇,王郑,朱垠光,等.2016.活性炭的再生方法比较及其发展趋势研究[J].化工技术与开发,45(10):44-48
侯立安,左莉.2003.二硫化碳的污染特征与净化材料的筛选试验[J].洁净与空调技术,(2):35-37
Karanfil T,Dastgheib S A.2004.Trichloroethylene adsorption by fibrous and granular activated carbons:aqueous phase,gas phase,and water vapor adsorption studies[J].Environmental Science&Technology,38(22):5834
Li L,Quinlivan P A,Knappe D R U.2002.Effects of activated carbon surface chemistry and pore structure on the adsorption of organic contaminants from aqueous solution[J].Carbon,40(12):2085-2100
李婷,王毅霖,张晓飞,等.2013.浅析活性炭再生技术的发展现状[C].中国环境科学学会2013年学术年会.昆明:6791-6793
Liang C,Bruell C.2008.Thermally activated persulfate oxidation of trichloroethylene:Experimental investigation of reaction orders[J].Industrial&Engineering Chemistry Research,47(9):2912-2918
Liang C,Lin Y T,Shin W H.2009a.Persulfate regeneration of trichloroethylene spent activated carbon[J].Journal of Hazardous Materials,168(1):187-192
Liang C,Su H W.2009b.Identification of sulfate and hydroxyl radicals in thermally activated persulfate[J].Industrial&Engineering Chemistry Research,48(11):472-475
刘守新,王岩,郑文超.2001.活性炭再生技术研究进展[J].东北林业大学学报,29(3):61-63
Narbaitz R M,Cen J.1997.Alternative methods for determining the percentage regeneration of activated carbon[J].Water Research,31(31):2532-2542
Quinlivan P A,Li L,Knappe D R.2005.Effects of activated carbon characteristics on the simultaneous adsorption of aqueous organic micropollutants and natural organic matter[J].Water Research,39(8):1663-1673
Rey A,Faraldos M,Casas J A,et al.2009.Catalytic wet peroxide oxidation of phenol over Fe/AC catalysts:Influence of iron precursor and activated carbon surface[J].Applied Catalysis B Environmental,86(1/2):69-77
Su Y F,Cheng Y L,Shih Y H.2013.Removal of trichloroethylene by zerovalent iron/activated carbon derived from agricultural wastes.[J].Journal of Environmental Management,129(129C):361-366
谭德俊,赵旭好,陈泉源.2014.基于硫酸根自由基的高级氧化技术原位再生活性炭[J].东华大学学报(自然科学版),40(5):633-638
王宝庆,陈亚雄,宁平.2000.活性炭水处理技术应用[J].环境科学导刊,19(3):46-49
王福禄.2011.Fenton试剂再生活性炭的试验研究[J].工业用水与废水,42(3):48-51
翁元声.2004.活性炭再生及新技术研究[J].给水排水,30(1):86-91
吴琪,宋乾武,曾燕艳,等.2011.活性炭再生技术研究进展和发展趋势[J].中国环保产业,(10):14-17
许伟,刘军利,孙康.2016.活性炭吸附法在挥发性有机物治理中的应用研究进展[J].化工进展,35(4):1223-1229
徐翯,冯流.2006.三氯乙烯在天然土壤中的吸附行为及其影响因素[J].农业环境科学学报,25(s1):65-68
Yamashita T,Hayes P.2008.Analysis of XPS spectra of Fe2+,and Fe3+,ions in oxide materials[J].Applied Surface Science,254(8):2441-2449
Yan N,Liu F,Xue Q,et al.2015.Degradation of trichloroethene by siderite-catalyzed hydrogen peroxide and persulfate:Investigation of reaction mechanisms and degradation products[J].Chemical Engineering Journal,274:61-68
曾雪玲,唐晓东,卢涛.2008.活性炭再生技术的研究进展[J].四川化工,11(4):11-15
周琴,沈健,黄敏.2013.活性炭的制备及再生研究进展[J].化学与生物工程,30(12):10-13