4种常用铁基材料非均相芬顿降解四环素的研究
|
摘要
为了筛选出成本低廉且快速有效的非均相芬顿催化剂,对比了Fe~0、Fe_3O_4、Fe_2O_3、α-FeOOH等4种常见非均相催化剂对四环素的去除效果;通过比表面积分析仪(BET)、激光粒度仪(LDI)分析了4种材料的理化特性;探究了4种材料的质量浓度、双氧水浓度、反应体系初始p H的影响,对比研究了4种材料非均相芬顿降解四环素的反应动力学,结果表明:Fe0不仅催化降解效果最好(对四环素的降解率为88.77%)、具有更宽的p H适用范围,而且价格低廉;最后,结合4种材料非均相芬顿降解四环素的TOC去除率、重复利用效率对比分析、荧光光谱法分析,最终筛选出Fe0为非均相芬顿降解四环素的最佳催化剂.
In order to screen out the low-cost,rapid and effective heterogeneous Fenton catalysts,the effects of four common heterogenous catalysts on Fe~0,Fe_3O_4,Fe_2O_3,and α-FeOOH were compared to remove tetracycline.The physicochemical properties of four materials were characterized with Brunnaer-Emmett-Teller( BET) surface area analyzer and laser particle size analyzer( LDI). The optimum reaction conditions were selected according to the effects of the four catalysts concentration,hydrogen peroxide concentration and initial pH. The kinetics of removal tetracycline was studied by comparing the four heterogeneous Fenton catalysts. The result showed that Fe0 is the best catalytic for degradation of tetracycline( 88.77% of tetracycline was removed),which is suitable for a wide range of pH in the reaction and low prices. In addition,the removal efficiency of the total organic carbon,reusability,fluorescent spectrometry was studied by comparing the four heterogeneous Fenton catalysts. Finally,Fe0 was selected to be the best catalyst for heterogeneous Fenton degradation of tetracycline.
In order to screen out the low-cost,rapid and effective heterogeneous Fenton catalysts,the effects of four common heterogenous catalysts on Fe~0,Fe_3O_4,Fe_2O_3,and α-FeOOH were compared to remove tetracycline.The physicochemical properties of four materials were characterized with Brunnaer-Emmett-Teller( BET) surface area analyzer and laser particle size analyzer( LDI). The optimum reaction conditions were selected according to the effects of the four catalysts concentration,hydrogen peroxide concentration and initial pH. The kinetics of removal tetracycline was studied by comparing the four heterogeneous Fenton catalysts. The result showed that Fe0 is the best catalytic for degradation of tetracycline( 88.77% of tetracycline was removed),which is suitable for a wide range of pH in the reaction and low prices. In addition,the removal efficiency of the total organic carbon,reusability,fluorescent spectrometry was studied by comparing the four heterogeneous Fenton catalysts. Finally,Fe0 was selected to be the best catalyst for heterogeneous Fenton degradation of tetracycline.
引文
[1] BAUTISTA P,MOHEDANO A F,CASAS J A,et al. An overview of the application of Fenton oxidation to industrial wastewaters treatment[J]. Journal of Chemical Technology&Biotechnology,2008,83(10):1323-1338.
[2] TRAPIOO M,KOLIK N,GOI A,et al. Fenton treatment efficacy for the purification of different kinds of wastewater[J]. Water Science&Technology:A Journal of the International Association on Water Pollution Research,2009,60(7):1795-1801.
[3]郭长征.多相芬顿法催化降解有机污染物进展[J].中国环境管理干部学院学报,2015(4):56-59.GUO C Z. Progress of catalytic degrading organic pollutants using heterogeneous fenton process[J]. Journal of EMCC,2015(4):56-59.
[4]张潇逸,何青春,蒋进元,等.类芬顿处理技术研究进展综述[J].环境科学与管理,2015(6):58-61.ZHANG X Y,HE Q C,JIANG J Y,et al. Study progress of class-fenton treatment technology[J]. Environmental Science and Management,2015(6):58-61.
[5]邓景衡,文湘华,李佳喜.碳纳米管负载纳米四氧化三铁多相类芬顿降解亚甲基蓝[J].环境科学学报,2014,34(6):1436-1442.DENG J H,WEN X H,LI J X. Degradation of methylene blue by heterogeneous Fenton-like reaction using Fe3O4/carbon nanotube composites[J]. Acta Scientiae Circumstantiae,2015(6):58-61.
[6]林光辉,吴锦华,李平,等.零价铁与双氧水异相Fenton降解活性艳橙X-GN[J].环境工程学报,2013,7(3):913-917.LIN G H,WU J H,LI P,et al. Effective degradation of reactive brilliant orange X-GN by heterogeneous Fenton reaction using zero-valent iron and H2O2[J]. Chinese Journal of Environmental Engineering,2013,7(3):913-917.
[7] VELICHKOVA F,JULCOUR-LEBIGUE C,KOUMANOVA B,et al. Heterogeneous Fenton oxidation of paracetamol using iron oxide(nano)particles[J]. Journal of Environmental Chemical Engineering,2013,1(4):1214-1222.
[8] RUI C M,LOPES D V,QUINA M J,et al. Treatment improvement of urban landfill leachates by Fenton-like process using ZVI[J]. Chemical Engineering Journal,2012,192(2):219-225.
[9] HUANG R,FANG Z,YAN X,et al. Heterogeneous sonoFenton catalytic degradation of bisphenol A by Fe3O4,magnetic nanoparticles under neutral condition[J].Chemical Engineering Journal,2012,197(14):242-249.
[10] GUADALUPE B,de la PLATA O,ORLANDO M,et al.Decomposition of 2-chlorophenol employing goethite as Fenton catalyst:I:proposal of a feasible,combined reaction scheme of heterogeneous and homogeneous reactions[J]. Applied Catalysis B:Environmental,2010,95(1/2):1-13.
[11] TAN L,LU S,FANG Z,et al. Enhanced reductive debromination and subsequent oxidative ring-opening of decabromodiphenyl ether by integrated catalyst of n ZVI supported on magnetic Fe3O4,nanoparticles[J]. Applied Catalysis B:Environmental,2017,200:200-210.
[12] AI Z H,LU L R,LI J P,et al. Fe@Fe2O3core-shell nanowires as iron reagent:1:efficient degradation of rhodamine B by a novel sono-Fenton process[J]. Journal of Physical Chemistry C,2007,111(11):4087-4093.
[13] RIVERA-UTRILLA J,GMEZ-PACHECO C V,SNCHEZ-POLO M,et al. Tetracycline removal from water by adsorption/bioadsorption on activated carbons and sludge-derived adsorbents[J]. Journal of Environmental Management,2013,131:16-24.
[14] KASPRZYK-HORDERN B,DINSDALE R M,GUWY A J. The occurrence of pharmaceuticals,personal care products,endocrine disruptors and illicit drugs in surface water in South Wales,UK[J]. Water Research,2008,42(13):3498-3518.
[15] LAPWORTH D J,BARAN N,STUART M E,et al. Emerging organic contaminants in groundwater:a review of sources,fate and occurrence[J]. Environmental Pollution,2012,163(4):287-303.
[16] JONES O A,LESTER J N,VOULVOULIS N. Pharmaceuticals:a threat to drinking water?[J]. Trends in Biotechnology,2005,23(4):163-167.
[17] SHARMA V K,JOHNSON N,CIZMAS L,et al. A review of the influence of treatment strategies on antibiotic resistant bacteria and antibiotic resistance genes[J]. Chemosphere,2016,150(3):702-714.
[18] HAO R,XIAO X,ZUO X,et al. Efficient adsorption and visible-light photocatalytic degradation of tetracycline hydrochloride using mesoporous Bi OI microspheres[J].Journal of Hazardous Materials,2012,209/210(1):137-145.
[19] GMEZ-PACHECO C V,SNCHEZ-POLO M,RIVERA-UTRILLA J,et al. Tetracycline degradation in aqueous phase by ultraviolet radiation[J]. Chemical Engineering Journal,2012,187(2):89-95.
[20]蒋胜韬,祝建中,管玉江,等. Si-Fe OOH/H2O2类芬顿降解盐酸四环素废水的效能及其机理[J].化工学报,2015,66(10):4244-4251.JIANG S T,ZHU J Z,GUAN Y J,et al. Degradation and mechanism of tetracycline hydrochloride in wastewater by Si-Fe OOH/H2O2Fenton-like[J]. CIESC Journal,2015,66(10):4244-4251.
[21]俞幼萍,高品,刘保江,等.新型光-类芬顿催化剂纳米Fe VO4的制备及其对盐酸四环素的降解性能[J].环境工程学报,2017,11(1):401-407.YU Y P,GAO P,LIU B J,et al. Preparation and degradation properties toward tetracycline hydrochloride of a new photo-Fenton-like catalyst nano Fe VO4[J]. Chinese Journal of Environmental Engineering,2017,11(1):401-407.
[22] KAKAVANDI B,TAKDASTAN A,JAAFARZADEH N,et al. Application of Fe3O4@C catalyzing heterogeneous UV-Fenton system for tetracycline removal with a focus on optimization by a response surface method[J]. Journal of Photochemistry and Photobiology A:Chemistry,2016,314(1):178-188.
[23] HOU L,WANG L,ROYER S,et al. Ultrasound-assisted heterogeneous Fenton-like degradation of tetracycline over a magnetite catalyst[J]. Journal of Hazardous Materials,2016,302:458-67.
[24] LIU S,ZHAO X R,SUN H Y,et al. The degradation of tetracycline in a photo-electro-Fenton system[J]. Chemical Engineering Journal,2013,231(9):441-448.
[2] TRAPIOO M,KOLIK N,GOI A,et al. Fenton treatment efficacy for the purification of different kinds of wastewater[J]. Water Science&Technology:A Journal of the International Association on Water Pollution Research,2009,60(7):1795-1801.
[3]郭长征.多相芬顿法催化降解有机污染物进展[J].中国环境管理干部学院学报,2015(4):56-59.GUO C Z. Progress of catalytic degrading organic pollutants using heterogeneous fenton process[J]. Journal of EMCC,2015(4):56-59.
[4]张潇逸,何青春,蒋进元,等.类芬顿处理技术研究进展综述[J].环境科学与管理,2015(6):58-61.ZHANG X Y,HE Q C,JIANG J Y,et al. Study progress of class-fenton treatment technology[J]. Environmental Science and Management,2015(6):58-61.
[5]邓景衡,文湘华,李佳喜.碳纳米管负载纳米四氧化三铁多相类芬顿降解亚甲基蓝[J].环境科学学报,2014,34(6):1436-1442.DENG J H,WEN X H,LI J X. Degradation of methylene blue by heterogeneous Fenton-like reaction using Fe3O4/carbon nanotube composites[J]. Acta Scientiae Circumstantiae,2015(6):58-61.
[6]林光辉,吴锦华,李平,等.零价铁与双氧水异相Fenton降解活性艳橙X-GN[J].环境工程学报,2013,7(3):913-917.LIN G H,WU J H,LI P,et al. Effective degradation of reactive brilliant orange X-GN by heterogeneous Fenton reaction using zero-valent iron and H2O2[J]. Chinese Journal of Environmental Engineering,2013,7(3):913-917.
[7] VELICHKOVA F,JULCOUR-LEBIGUE C,KOUMANOVA B,et al. Heterogeneous Fenton oxidation of paracetamol using iron oxide(nano)particles[J]. Journal of Environmental Chemical Engineering,2013,1(4):1214-1222.
[8] RUI C M,LOPES D V,QUINA M J,et al. Treatment improvement of urban landfill leachates by Fenton-like process using ZVI[J]. Chemical Engineering Journal,2012,192(2):219-225.
[9] HUANG R,FANG Z,YAN X,et al. Heterogeneous sonoFenton catalytic degradation of bisphenol A by Fe3O4,magnetic nanoparticles under neutral condition[J].Chemical Engineering Journal,2012,197(14):242-249.
[10] GUADALUPE B,de la PLATA O,ORLANDO M,et al.Decomposition of 2-chlorophenol employing goethite as Fenton catalyst:I:proposal of a feasible,combined reaction scheme of heterogeneous and homogeneous reactions[J]. Applied Catalysis B:Environmental,2010,95(1/2):1-13.
[11] TAN L,LU S,FANG Z,et al. Enhanced reductive debromination and subsequent oxidative ring-opening of decabromodiphenyl ether by integrated catalyst of n ZVI supported on magnetic Fe3O4,nanoparticles[J]. Applied Catalysis B:Environmental,2017,200:200-210.
[12] AI Z H,LU L R,LI J P,et al. Fe@Fe2O3core-shell nanowires as iron reagent:1:efficient degradation of rhodamine B by a novel sono-Fenton process[J]. Journal of Physical Chemistry C,2007,111(11):4087-4093.
[13] RIVERA-UTRILLA J,GMEZ-PACHECO C V,SNCHEZ-POLO M,et al. Tetracycline removal from water by adsorption/bioadsorption on activated carbons and sludge-derived adsorbents[J]. Journal of Environmental Management,2013,131:16-24.
[14] KASPRZYK-HORDERN B,DINSDALE R M,GUWY A J. The occurrence of pharmaceuticals,personal care products,endocrine disruptors and illicit drugs in surface water in South Wales,UK[J]. Water Research,2008,42(13):3498-3518.
[15] LAPWORTH D J,BARAN N,STUART M E,et al. Emerging organic contaminants in groundwater:a review of sources,fate and occurrence[J]. Environmental Pollution,2012,163(4):287-303.
[16] JONES O A,LESTER J N,VOULVOULIS N. Pharmaceuticals:a threat to drinking water?[J]. Trends in Biotechnology,2005,23(4):163-167.
[17] SHARMA V K,JOHNSON N,CIZMAS L,et al. A review of the influence of treatment strategies on antibiotic resistant bacteria and antibiotic resistance genes[J]. Chemosphere,2016,150(3):702-714.
[18] HAO R,XIAO X,ZUO X,et al. Efficient adsorption and visible-light photocatalytic degradation of tetracycline hydrochloride using mesoporous Bi OI microspheres[J].Journal of Hazardous Materials,2012,209/210(1):137-145.
[19] GMEZ-PACHECO C V,SNCHEZ-POLO M,RIVERA-UTRILLA J,et al. Tetracycline degradation in aqueous phase by ultraviolet radiation[J]. Chemical Engineering Journal,2012,187(2):89-95.
[20]蒋胜韬,祝建中,管玉江,等. Si-Fe OOH/H2O2类芬顿降解盐酸四环素废水的效能及其机理[J].化工学报,2015,66(10):4244-4251.JIANG S T,ZHU J Z,GUAN Y J,et al. Degradation and mechanism of tetracycline hydrochloride in wastewater by Si-Fe OOH/H2O2Fenton-like[J]. CIESC Journal,2015,66(10):4244-4251.
[21]俞幼萍,高品,刘保江,等.新型光-类芬顿催化剂纳米Fe VO4的制备及其对盐酸四环素的降解性能[J].环境工程学报,2017,11(1):401-407.YU Y P,GAO P,LIU B J,et al. Preparation and degradation properties toward tetracycline hydrochloride of a new photo-Fenton-like catalyst nano Fe VO4[J]. Chinese Journal of Environmental Engineering,2017,11(1):401-407.
[22] KAKAVANDI B,TAKDASTAN A,JAAFARZADEH N,et al. Application of Fe3O4@C catalyzing heterogeneous UV-Fenton system for tetracycline removal with a focus on optimization by a response surface method[J]. Journal of Photochemistry and Photobiology A:Chemistry,2016,314(1):178-188.
[23] HOU L,WANG L,ROYER S,et al. Ultrasound-assisted heterogeneous Fenton-like degradation of tetracycline over a magnetite catalyst[J]. Journal of Hazardous Materials,2016,302:458-67.
[24] LIU S,ZHAO X R,SUN H Y,et al. The degradation of tetracycline in a photo-electro-Fenton system[J]. Chemical Engineering Journal,2013,231(9):441-448.