石墨烯泡沫包裹铁电极的制备及其在电解脱色染料中的应用研究
|
摘要
通过水热还原氧化石墨烯在铁电极表面原位生长石墨烯泡沫的方法制得了石墨烯泡沫包裹铁电极(GS-Fe电极),并将其应用于多种染料的电解脱色。结果表明:在相同电流密度下,GS-Fe电极的电解反应速率常数是铁电极的5倍;加入电解质对电解效率至关重要,其中NaCl是最有效的电解质;对甲烯蓝而言,最佳的电解条件为甲烯蓝初始质量浓度30mg/L、pH 5~7;GS-Fe电极可用于电解脱色刚果红、酸性蓝92和活性蓝R。电解脱色的机制推测主要为间接氧化,Cl~-被氧化成ClO~-,而后ClO~-氧化染料。GS-Fe电极可通过简单清洗再生,电解的脱色率几乎不受影响。
By hydrothermal reduction of graphene oxide,graphene sponge was in situ coated on the surface of Fe electrode to obtain GS coated Fe electrode(GS-Fe electrode),which was used in the electrolytic decoloration of various dyes.The data indicated that:the decoloration kinetics constant of GS-Fe electrode was five times of that of Fe electrode at the same current density.The presence of electrolyte was crucial for the electrolysis,among which NaCl was the most effective one.The optimal electrolysis conditions were at methylene blue(MB)concentration of 30 mg/L and pH 5-7.GS-Fe electrode could also be applied in the electrolytic decoloration of congo red,acidic blue 92 and remazol brilliant blue R.The possible electrolytic decoloration mechanism was speculated as indirect oxidation,where Clwas oxidized into ClO~-for the oxidation of dyes.GS-Fe electrode could be regenerated by simple washing and the decoloration efficiency was not influenced.
By hydrothermal reduction of graphene oxide,graphene sponge was in situ coated on the surface of Fe electrode to obtain GS coated Fe electrode(GS-Fe electrode),which was used in the electrolytic decoloration of various dyes.The data indicated that:the decoloration kinetics constant of GS-Fe electrode was five times of that of Fe electrode at the same current density.The presence of electrolyte was crucial for the electrolysis,among which NaCl was the most effective one.The optimal electrolysis conditions were at methylene blue(MB)concentration of 30 mg/L and pH 5-7.GS-Fe electrode could also be applied in the electrolytic decoloration of congo red,acidic blue 92 and remazol brilliant blue R.The possible electrolytic decoloration mechanism was speculated as indirect oxidation,where Clwas oxidized into ClO~-for the oxidation of dyes.GS-Fe electrode could be regenerated by simple washing and the decoloration efficiency was not influenced.
引文
[1]WU Changhua,MAURER C,WANG Yi,et al.Water pollution and human health in China[J].Environ.Health Perspect.,1999,107(4):251-256.
[2]刘雅玲,王强,吴悦颖,等.纺织行业水污染物排放量的关键影响要素研究[J].环境污染与防治,2015,37(3):58-61.
[3]ROBINSON T,MCMULLAN G,MARCHANT R,et al.Remediation of dyes in textile effluent:a critical review on current treatment technologies with a proposed alternative[J].Bioresour.Technol.,2001,77(3):247-255.
[4]MOHAN D,PITTMAN C.Activated carbons and low cost adsorbents for remediation of tri-and hexavalent chromium from water[J].J.Hazard.Mater.,2006,137(2):762-811.
[5]孙南南,谢实涛,李凯,等.RuO2-IrO2-SnO2/Ti阳极电催化氧化苯酚的研究[J].环境污染与防治,2015,37(2):38-41.
[6]SIRES I,BRILLAS E.Remediation of water pollution caused by pharmaceutical residues based on electrochemical separation and degradation technologies:a review[J].Environ.Int.,2012,40:212-229.
[7]VANDEVIVERE P,BIANCHI R,VERSTRAETE W.Treatment and reuse of wastewater from the textile wet-processing industry:review of emerging technologies[J].Chem.Technol.Biotechnol.,1998,72(4):289-302.
[8]ZHANG Yifeng,ANGELIDAKI I.Microbial electrolysis cells turning to be versatile technology:recent advances and future challenges[J].Water Res.,2014,56(3):11-25.
[9]SIRES I,BRILLAS E,RODRIGO M,et al.Electrochemical advanced oxidation processes:today and tomorrow.A review[J].Environ.Sci.Pollut.Res.,2014,21(14):8336-8367.
[10]PULKKA S,MARTIKAINEN M,BHATNAGAR A,et al.Electrochemical methods for the removal of anionic contaminants from water-a review[J].Sep.Purif.Technol.,2014,132:252-271.
[11]王瑞珏,刘潇阳,张孝亮,等.四氧化三铁-石墨烯复合芬顿催化剂用于染料脱色的研究[J].西南民族大学学报(自然科学版),2015,41(5):588-592.
[12]杨胜韬,赵连勤.石墨烯吸附材料的制备与应用研究进展[J].西南民族大学学报(自然科学版),2014,40(2):203-218.
[13]FUJII S,ENOKI T.Nanographene and graphene edges:electronic structure and nanofabrication[J].Acc.Chem.Res.,2013,46(10):2202-2210.
[14]LU Meijiao,LI Jing,YANG Xuyu,et al.Applications of graphene-based materials in environmental protection and detection[J].Sci.Bull.,2013,58(22):2698-2710.
[15]MA Xuemei,MIAO Tingting,ZHU Wencai,et al.Electrochemical detection of nitrite based on glassy carbon electrode modified with gold-polyaniline-graphene nanocomposites[J].RSC Adv.,2014,101(4):57842-57849.
[16]LIU Yanbiao,LEE J,XIA Qing,et al.A graphene-based electrochemical filter for water purification[J].J.Mater.Chem.A,2014,39(2):16554-16562.
[17]ZHAI Chunyang,ZHU Mingshan,REN Fangfang,et al.Enhanced photoelectrocatalytic performance of titanium dioxide/carbon cloth based photoelectrodes by graphene modification under visible-light irradiation[J].J.Hazard.Mater.,2013,263:291-298.
[18]TOVIDE O,JAHED N,SUNDAY C,et al.Electro-oxidation of anthracene on polyanilino-graphene composite electrode[J].Sensors&Actuators B Chemical,2014,205(4):184-192.
[19]ZHAO Lianqin,YU Baowei,XUE Fumin,et al.Facile hydrothermal preparation of recyclable S-doped graphene sponge for Cu2+adsorption[J].J.Hazard.Mater.,2015,286:449-456.
[20]赵连勤,张孝亮,谢静茹,等.水热法制备三氧化二铝掺杂石墨烯泡沫[J].西南民族大学学报(自然科学版),2014,40(6):849-852.
[21]WANG Jialiang,SHI Zixing,FAN Jinchen,et al.Self-assembly of graphene into three-dimensional structures promoted by natural phenolic acids[J].J.Mater.Chem.,2012,22(42):22459-22466.
[22]YANG Shengtao,CHANG Yanli,WANG Haifang,et al.Folding/aggregation of graphene oxide and its application in Cu2+removal[J].Journal of Colloid and Interface Science,2010,351(1):122-127.
[23]张亚静,应金英,陈晓锋.铁碳内电解法处理印染废水[J].环境导报,2000,22(5):33-36.
[2]刘雅玲,王强,吴悦颖,等.纺织行业水污染物排放量的关键影响要素研究[J].环境污染与防治,2015,37(3):58-61.
[3]ROBINSON T,MCMULLAN G,MARCHANT R,et al.Remediation of dyes in textile effluent:a critical review on current treatment technologies with a proposed alternative[J].Bioresour.Technol.,2001,77(3):247-255.
[4]MOHAN D,PITTMAN C.Activated carbons and low cost adsorbents for remediation of tri-and hexavalent chromium from water[J].J.Hazard.Mater.,2006,137(2):762-811.
[5]孙南南,谢实涛,李凯,等.RuO2-IrO2-SnO2/Ti阳极电催化氧化苯酚的研究[J].环境污染与防治,2015,37(2):38-41.
[6]SIRES I,BRILLAS E.Remediation of water pollution caused by pharmaceutical residues based on electrochemical separation and degradation technologies:a review[J].Environ.Int.,2012,40:212-229.
[7]VANDEVIVERE P,BIANCHI R,VERSTRAETE W.Treatment and reuse of wastewater from the textile wet-processing industry:review of emerging technologies[J].Chem.Technol.Biotechnol.,1998,72(4):289-302.
[8]ZHANG Yifeng,ANGELIDAKI I.Microbial electrolysis cells turning to be versatile technology:recent advances and future challenges[J].Water Res.,2014,56(3):11-25.
[9]SIRES I,BRILLAS E,RODRIGO M,et al.Electrochemical advanced oxidation processes:today and tomorrow.A review[J].Environ.Sci.Pollut.Res.,2014,21(14):8336-8367.
[10]PULKKA S,MARTIKAINEN M,BHATNAGAR A,et al.Electrochemical methods for the removal of anionic contaminants from water-a review[J].Sep.Purif.Technol.,2014,132:252-271.
[11]王瑞珏,刘潇阳,张孝亮,等.四氧化三铁-石墨烯复合芬顿催化剂用于染料脱色的研究[J].西南民族大学学报(自然科学版),2015,41(5):588-592.
[12]杨胜韬,赵连勤.石墨烯吸附材料的制备与应用研究进展[J].西南民族大学学报(自然科学版),2014,40(2):203-218.
[13]FUJII S,ENOKI T.Nanographene and graphene edges:electronic structure and nanofabrication[J].Acc.Chem.Res.,2013,46(10):2202-2210.
[14]LU Meijiao,LI Jing,YANG Xuyu,et al.Applications of graphene-based materials in environmental protection and detection[J].Sci.Bull.,2013,58(22):2698-2710.
[15]MA Xuemei,MIAO Tingting,ZHU Wencai,et al.Electrochemical detection of nitrite based on glassy carbon electrode modified with gold-polyaniline-graphene nanocomposites[J].RSC Adv.,2014,101(4):57842-57849.
[16]LIU Yanbiao,LEE J,XIA Qing,et al.A graphene-based electrochemical filter for water purification[J].J.Mater.Chem.A,2014,39(2):16554-16562.
[17]ZHAI Chunyang,ZHU Mingshan,REN Fangfang,et al.Enhanced photoelectrocatalytic performance of titanium dioxide/carbon cloth based photoelectrodes by graphene modification under visible-light irradiation[J].J.Hazard.Mater.,2013,263:291-298.
[18]TOVIDE O,JAHED N,SUNDAY C,et al.Electro-oxidation of anthracene on polyanilino-graphene composite electrode[J].Sensors&Actuators B Chemical,2014,205(4):184-192.
[19]ZHAO Lianqin,YU Baowei,XUE Fumin,et al.Facile hydrothermal preparation of recyclable S-doped graphene sponge for Cu2+adsorption[J].J.Hazard.Mater.,2015,286:449-456.
[20]赵连勤,张孝亮,谢静茹,等.水热法制备三氧化二铝掺杂石墨烯泡沫[J].西南民族大学学报(自然科学版),2014,40(6):849-852.
[21]WANG Jialiang,SHI Zixing,FAN Jinchen,et al.Self-assembly of graphene into three-dimensional structures promoted by natural phenolic acids[J].J.Mater.Chem.,2012,22(42):22459-22466.
[22]YANG Shengtao,CHANG Yanli,WANG Haifang,et al.Folding/aggregation of graphene oxide and its application in Cu2+removal[J].Journal of Colloid and Interface Science,2010,351(1):122-127.
[23]张亚静,应金英,陈晓锋.铁碳内电解法处理印染废水[J].环境导报,2000,22(5):33-36.