微波催化剂MgFe_2O_4-Fe_2O_3微波催化氧化降解结晶紫废水
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摘要
提出一种新型的、无需添加氧化剂处理结晶紫废水的方法.通过共沉淀晶化法制备微波催化剂MgFe_2O_4-Fe_2O_3,在微波辐照下降解结晶紫废水,考察了催化剂用量、微波功率、辐照时间对结晶紫去除率的影响.结果表明:在一定条件下,去除率随着催化剂用量的增加、微波功率的增大、微波辐照时间的延长而增加.当微波功率为800 W,辐照时间5min,催化剂用量1g/L时,处理200mg/L的结晶紫废水,去除率可达99.3%.本文还对微波催化氧化机理进行了探究,通过添加不同氧化基团清除剂的实验发现,氧化基团清除剂的添加降低了结晶紫的去除率,并提出了该反应的微观机理:微波催化剂吸收电磁波发生光电效应,产生电子和空穴对,与水等作用产生·OH,·OH再氧化降解废水中的有机物.
A new degradation method for crystal violet(CV)from wastewater was proposed without adding any oxidant.The microwave catalyst of MgFe_2O_4-Fe_2O_3 was obtained through co-precipitation crystallization method,and its degradation performance for the wastewater containing CV was systematically evaluated under microwave irradiation,including catalyst dosage,microwave power and irradiation time.The results indicated that microwave catalyst MgFe_2O_4-Fe_2O_3 displayes excellent catalytic activity,and degradation efficiency for CV from a 200 mg/L wastewater can be highly up to 99.3% with microwave power of 800 W,catalyst dosage of 1g/L,and irradiation time of 5min.In addition,the mechanism for the microwave catalytic oxidation degradation was preliminary discussed,and hydroxyl radical(·OH)generated during the catalytic reaction acted as the dominant oxidant for the degradation,demonstrating from the experiment of adding different oxides as removal agents.Under microwave irradiation,microwave catalyst can effectively absorb electromagnetic wave to produce photo-electric effects with generation of electron-hole pairs(e-cb+h+vb),which will react with H_2O molecules to produce·OH,and then the formed·OH groups oxidation can degrade the organic compounds existing in wastewater.The proposed microwave catalytic oxidation degradation is a new method for highly efficient degradation of organic wastewater.
A new degradation method for crystal violet(CV)from wastewater was proposed without adding any oxidant.The microwave catalyst of MgFe_2O_4-Fe_2O_3 was obtained through co-precipitation crystallization method,and its degradation performance for the wastewater containing CV was systematically evaluated under microwave irradiation,including catalyst dosage,microwave power and irradiation time.The results indicated that microwave catalyst MgFe_2O_4-Fe_2O_3 displayes excellent catalytic activity,and degradation efficiency for CV from a 200 mg/L wastewater can be highly up to 99.3% with microwave power of 800 W,catalyst dosage of 1g/L,and irradiation time of 5min.In addition,the mechanism for the microwave catalytic oxidation degradation was preliminary discussed,and hydroxyl radical(·OH)generated during the catalytic reaction acted as the dominant oxidant for the degradation,demonstrating from the experiment of adding different oxides as removal agents.Under microwave irradiation,microwave catalyst can effectively absorb electromagnetic wave to produce photo-electric effects with generation of electron-hole pairs(e-cb+h+vb),which will react with H_2O molecules to produce·OH,and then the formed·OH groups oxidation can degrade the organic compounds existing in wastewater.The proposed microwave catalytic oxidation degradation is a new method for highly efficient degradation of organic wastewater.
引文
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[26]ZHENG W X,MAYRIN M,A TARR M.Enhancement of sonochemical degradation of phenol using hydrogen atom scavengers[J].Ultrason Sonochem,2005,12(4):313-317.
[27]GUO Yu-wei,CHENG Chun-ping,WANG Jun,et al.Detection of reactive oxygen species(ROS)generated by TiO2(R),TiO2(R/A)and TiO2(A)under ultrasonic and solar light irradiation and application indegradation of organic dyes[J].Journal of Hazardous Materials,2011,192:786-793.
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[2]KAMBOH M A,SOLANGI I B,SHERAZI S T H,et al.A highly efficient calyx arene based resin for the removal of azo dyes[J].Desalination,2011,268(1/3):83-89.
[3]GOLKA K,KOPPS S,MYSLAK Z W.Carcinogenicity of azo colorants:Influence of solubility and bioavailability[J].Toxicol Lett,2004,151(1):203-210.
[4]NASSAR M M,MAGDY Y H.Removal of different basic dyes from aqueous solutions by adsorption on palm-fruit bunch particles[J].Chem Eng J,1997,66(3):223-226.
[5]CHAKRABORTY S,CHOWDHURY S,DAS P S.Adsorption of crystal violet from aqueous solution onto NaOH-modified rice husk[J].Carbohydr Polym,2011,86(4):1533-1541.
[6]PARSHETTI G K,PARSHETTI S G,TELKE A A,et al.Biodegradation of crystal violet by agrobacterium radiobacter[J].Environ Sci,2011,23(8):1384-1393.
[7]FERNANDO G D,CHRISTIAN P,CESAR P,et al.Torres-palma.effects of sonochemical parameters and inorganic ions during the sonochemical degradation of crystal violet in water[J].Ultrason Sonochem,2011,18(1):440-446.
[8]张文治,张秀丽,李莉,等.CTAB作用下纳米复合材料ZnOTiO2制备与多模式光催化降解罗丹明B[J].分子催化,2013,27(5):474-482.ZHANG Wen-zhe,ZHANG Xiu-li,LI li,et al.The preparation of nanocomposite ZnO-TiO2by CTAB-sssisted synthesis and multi-mode photo-catalytic degradation of rhodamine B[J].J Molecular Catalysis,2013,27(5):474-482.(In Chinese)
[9]因博,龙东辉,徐伟,等.板式纳米碳纤维负载二氧化钛光催化复合材料的制备及降解甲基橙的研究[J].分子催化,2012,26(5):442-448.YIN Bo,LONG Dong-hui,XU Wei,et al.Preparation of TiO2/Platelet carbon nanofiber nanocomposites and their photo-catalytic performance for degradation of methyl orange[J].J Molecular Catalysis,2012,26(5):442-448.(In Chinese)
[10]RICARDO E,GOYES P,FERNANDO L,et al.Electrochemical degradation of crystal violet with BDD electrodes:Effect of electrochemical parameters and identification of organic by-products[J].Chemosphere,2010,81(1):26-32.
[11]JANA S,PURKAIT M K,MOHANTY K.Removal of crystal violet by advanced oxidation and microfiltration[J].Applied Clay Science,2010,50(3):337-341.
[12]SZYMAN′SKI G S.Catalytic destruction of methyl tertiary butyl ether(MTBE)using oxidized carbon[J].Catal Today,2008,137(2):460-465.
[13]LIN L,YUAN S H,CHEN J,et al.Removal of ammonia nitrogen in wastewater by microwave radiation[J].J Hazard Mater,2009,161:(s2/3)1063-1068.
[14]ZHANG Z H,XU Y,MA X P,et al.Microwave degradation of methyl orange dye in aqueous solution in the presence of nano-TiO2-supported activated carbon(supported-TiO2/AC/MW)[J].J Hazard Mater,2012,209/210:271-277.
[15]HE H,YANG S,YU K,et al.Microwave induced catalytic degradation of crystal violet in nano-nickel dioxide suspensions[J].J Hazard Mater,2010,173(1/3):393-400.
[16]BI X,WANG P,JIAO C,et al.Degradation of remazol golden yellow dye wastewater in microwave enhanced ClO2catalytic oxidation process[J].J Hazard Mater,2009,168(2/3):895-900.
[17]LIU S T,ZHANG A B,YAN K K,et al.Microwave-enhanced catalytic degradation of methylene blue by porous MFe2O4(M=Mn,Co)nanocomposites:Pathways and mechanisms[J].Sep Purif Technol,2014,135:35-41.
[18]周继承,王哲,蒋尊芳,等.一种微波催化剂及应用方法:中国,102407113A[P].2012-04-11.ZHOU Ji-cheng,WANG Zhe,JIANG Zun-fang,et al.A microwave catalyst and its application method.Chinese,102407113A[P].2012-04-11.(In Chinese)
[19]周继承,蒋尊芳,高令飞,等.一种采用活性炭基微波催化剂降解有机废水的方法:中国,102992444A[P].2013-03-27.ZHOU Ji-cheng,JIANG Zun-fang,GAO Ling-fei,et al.A method for the degradation of organic wastewater by activated carbon microwave catalyst:Chinese,102992444A[P].2013-03-27.(In Chinese)
[20]周继承,蒋尊芳,高令飞,等.一种采用铁酸盐类微波催化剂降解有机废水的方法:中国,103011333A[P].2013-04-03.ZHOU Ji-cheng,JIANG Zun-fang,GAO Ling-fei,et al.A method for the degradation of organic wastewater by ferrite microwave catalyst:Chinese,103011333A[P].2013-04-03.(In Chinese)
[21]周继承,蒋尊芳,谌敏飞,等.一种降解有机废水的微波催化剂及其催化氧化降解方法:中国,103084216A[P].2013-05-08.ZHOU Ji-cheng,JIANG Zun-fang,ZHAN Mei-fei,et al.A microwave catalyst for the degradation of organic wastewater and its catalytic oxidation degradation:Chinese,103084216A[P].2013-05-08.(In Chinese)
[22]ZHANG L,LIU X Y,GUO X J,et al.Investigation on the degradation of brilliant green induced oxidation by NiFe2O4under microwave irradiation[J].Chem Eng J,2011,173(3):737-742.
[23]HONG Z C,SHAO G Y,JIAO C,et al.Efficient degradation of crystal violet in magnetic CuFe2O4aqueous solution coupled with microwave radiation[J].Chemosphere,2012,89(2):185-189.
[24]吁霁,庄稼,迟燕华,等.纳米ZnFe2O4的低温固相合成及其电磁损耗特性[J].材料科学与工程学报,2004,22(1):110-112.YU Ji,ZHUANG Jia,CHI Yan-hua,et al.Low temperature solid state synthesis of nano ZnFe2O4and characterization of its electromagnetic loss[J].J Mater Sci and Eng,2004,22(1):110-112.(In Chinese)
[25]GARGANTINI I.Further applications of circular arithmatic Schroedercike algorithms with error bovends for finding zeros of polynomials[J].SIAMJ,1998,15:497-510.
[26]ZHENG W X,MAYRIN M,A TARR M.Enhancement of sonochemical degradation of phenol using hydrogen atom scavengers[J].Ultrason Sonochem,2005,12(4):313-317.
[27]GUO Yu-wei,CHENG Chun-ping,WANG Jun,et al.Detection of reactive oxygen species(ROS)generated by TiO2(R),TiO2(R/A)and TiO2(A)under ultrasonic and solar light irradiation and application indegradation of organic dyes[J].Journal of Hazardous Materials,2011,192:786-793.
[28]QUAN X,ZHANG Y B,CHEN S,et al.Generation of hydroxyl radical in aqueous solution by microwave energy using activated carbon as catalyst and its potential in removal of persistent organic substances[J].J Mol Catal A:Chem,2007,263(1/2):216-222.
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