活性炭纤维三维电极电催化降解水中间甲酚——效能及影响因素研究
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摘要
探讨了以活性炭纤维作为三维粒子电极电氧化降解水中间甲酚的可行性与效果.首先对活性炭纤维的表面形貌,比表面积,孔结构和表面官能团情况进行了表征,发现活性炭纤维(ACFs)以单束纤维的结构交叉排列而成,比表面积较大(>1480m2/g),另外发现活性炭纤维的表面存在较多官能团种类.结合活性炭纤维表征结果,论文对活性炭纤维三维电极的相关影响因素进行了考察,研究了活性炭纤维种类,活性炭纤维与电极的接触方式以及反应溶液初始pH值对实验结果的影响.结果表明,活性炭纤维表面过多的含氧官能团不利于污染物的快速降解,而三维电极电氧化效果随着pH值的降低而显著增大,不同的电极接触方式对三维电极电氧化效果也有较大影响.
The feasibility and efficiency of m-cresol removal with three different categories of activated carbon fibers(ACFs) as particle electrodes were investigated. The surface morphology of activated carbon fibers was examined by scanning electron microscopy(SEM). The pore structure and specific surface area of activated carbon fibers were studied by BET. The variety and number of surface functional groups of activated carbon fibers were characterized by temperature programmed desorption(TPD-Ms). It was found the activated carbon fibers were formed by cro ss binding of single bundle fibers structure with a large specific surface area(>1480m2/g) and diverse functional groups. Furthermore, influence of operating parameters was investigated including the effects of ACFs types, contact mode of ACFs and electrode, as well as initial pH. The electrochemical degradation results demonstrated that the excessive oxygen functional groups on the surface of ACFs might be adverse to the removal rate of pollutants. The electrooxidation efficiency of three-dimensional electrodes increases significantly with the decrease of pH, and different electrode contact modes also have great influence on the electrooxidation effect of three-dimensional electrode.
The feasibility and efficiency of m-cresol removal with three different categories of activated carbon fibers(ACFs) as particle electrodes were investigated. The surface morphology of activated carbon fibers was examined by scanning electron microscopy(SEM). The pore structure and specific surface area of activated carbon fibers were studied by BET. The variety and number of surface functional groups of activated carbon fibers were characterized by temperature programmed desorption(TPD-Ms). It was found the activated carbon fibers were formed by cro ss binding of single bundle fibers structure with a large specific surface area(>1480m2/g) and diverse functional groups. Furthermore, influence of operating parameters was investigated including the effects of ACFs types, contact mode of ACFs and electrode, as well as initial pH. The electrochemical degradation results demonstrated that the excessive oxygen functional groups on the surface of ACFs might be adverse to the removal rate of pollutants. The electrooxidation efficiency of three-dimensional electrodes increases significantly with the decrease of pH, and different electrode contact modes also have great influence on the electrooxidation effect of three-dimensional electrode.
引文
[1]Liu P J,He S B,Wei H Z,et al.Characterization ofα-Fe2O3/γ-Al2O3catalysts for catalytic wet peroxide oxidation of m-cresol[J].Industrial&Engineering Chemistry Research,2015,54(1):130-136.
[2]GB 8978-1996污水综合排放标准[S].GB 8978-1996 Integrated wastewater discharge standard[S].
[3]Kennedy L J,Vijaya J J,Sekaran G,et al.Equilibrium,kinetic and thermodynamic studies on the adsorption of m-cresol onto micro10.1016/j.jhazmat.2007.03.061-and mesoporous carbon[J].Journal of Hazardous Materials,2007,149(1):134-143.
[4]Ahamad P Y A,Kunhi A A M.Degradation of high concentrations of cresols by Pseudomonas sp CP4[J].World Journal of Microbiology&Biotechnology,1999,15(2):321-323.
[5]Yu Y,Wei H Z,Yu L,et al.Catalytic wet air oxidation of m-cresol over a surface-modified sewage sludge-derived carbonaceous catalyst[J].Catalysis Science&Technology,2016,6(4):1085-1093.
[6]Yu Y,Wei H Z,Yu L,et al.Sewage-sludge-derived carbonaceous materials for catalytic wet hydrogen peroxide oxidation of m-cresol in batch and continuous reactors[J].Environmental Technology,2016,37(2):153-162.
[7]Zhou H,Guo J J,Li P,et al.Leaf-architectured 3D hierarchical artificial photosynthetic system of perovskite titanates towards CO2photoreduction into hydrocarbon fuels[J].Scientific Reports,2013,3.
[8]张小玲,班云霄.LED联合玻璃纤维光催化填料对苯酚的降解研究[J].中国环境科学,2018,38(8):2941-2946.Zhang X L,Ban Y X.Study on the degradation of phenol by UV-LEDcombined with glass fiber photocatalytic fillers[J].China Environmental Science,2018,38(8):2941-2946.
[9]Sires I,Brillas E,Oturan M A,et al.Electrochemical advanced oxidation processes:today and tomorrow.A review[J].Environmental Science and Pollution Research,2014,21(14):8336-8367.
[10]Hermosilla D,Merayo N,Gasco A,et al.The application of advanced oxidation technologies to the treatment of effluents from the pulp and paper industry:a review[J].Environmental Science and Pollution Research,2015,22(1):168-191.
[11]Xiong Y,He C,Karlsson H T,et al.Performance of three-phase three-dimensional electrode reactor for the reduction of COD in simulated wastewater-containing phenol[J].Chemosphere,2003,50(1):131-136.
[12]Xiong Y,He C,An T C,et al.Removal of formic acid from wastewater using three-phase three-dimensional electrode reactor[J].Water,Air,and Soil Pollution,2003,144(1):67-79.
[13]伍波,李鹏,张波,等.负载型粒子电极电催化氧化苯酚的研究[J].中国环境科学,2015,35(8):2426-2432.Wu B,Li P,Zhang B,et al.Electro-catalytic performance of the activated carbon supported metal oxide as particulate electrode for phenol oxidation[J].China Environmental Science,2015,35(8):2426-2432.
[14]Wu X B,Yang X Q,Wu D C,et al.Feasibility stud of using carbon aerogel as particle electrodes for decoloration of RBRX dye solution in a three-dimensional electrode reactor[J].Chemical Engineering Journal,2008,138(1-3):47-54.
[15]Boudenne J L,Cerclier O.Performance of carbon black-slurry electrodes for 4-chlorophenol oxidation[J].Water Research,1999,33(2):494-504.
[16]Sharifian H,Kirk D W.Electrochemical oxidation of phenol[J].Journal of the Electrochemical Society,1986,133(5):921-924.
[17]张芳,李光明,盛怡,等.电催化氧化法处理苯酚废水的Mn-SnSb/γ-Al2O3粒子电极研制[J].化学学报,2006,64(3):235-239.Zhang F,Li G M,Sheng Y,et al.Preparation of Mn-Sn-Sb/γ-Al2O3particle-electrodes for electrocatalytic oxidation of phenol wastewater[J].Acta Chimica Sinica,2006,64(3):235-239.
[18]Gu L,Wang B,Ma H Z,et al.Catalytic oxidation of anionic surfactants by electrochemical oxidation with Cu O-Co2O3-PO43-modified kaolin[J].Journal of Hazardous Materials,2006,137(2):842-848.
[19]Ma L,Sun C L,Ren J,et al.Efficient electrochemical incineration of phenol on activated carbon fiber as a new type of particulates[J].Russian Journal of Electrochemistry,2014,50(6):569-578.
[20]Chou W L,Wang C T,Chang C P.Comparison of removal of Acid Orange 7 by electrooxidation using various anode materials[J].Desalination,2011,266(1-3):201-207.
[21]Hueso J L,Espinós J P,Caballero A,et al.XPS investigation of the reaction of carbon with NO,O2,N2 and H2O plasmas[J].Carbon,2007,45(1):89-96.
[22]孙杰,钟超,彭巧丽.活性炭纤维复合阴极材料电芬顿降解苯酚[J].中南民族大学学报(自然科学版),2015,34(2):6.Sun J,Zhong C,Peng Q L.Electro-Fenton degradation of phenol using hybridized activated carbon fiber as cathode materials[J].Journal of SouthCentral University for Nationalities(Natural Science Edition),2015,34(2):6.
[2]GB 8978-1996污水综合排放标准[S].GB 8978-1996 Integrated wastewater discharge standard[S].
[3]Kennedy L J,Vijaya J J,Sekaran G,et al.Equilibrium,kinetic and thermodynamic studies on the adsorption of m-cresol onto micro10.1016/j.jhazmat.2007.03.061-and mesoporous carbon[J].Journal of Hazardous Materials,2007,149(1):134-143.
[4]Ahamad P Y A,Kunhi A A M.Degradation of high concentrations of cresols by Pseudomonas sp CP4[J].World Journal of Microbiology&Biotechnology,1999,15(2):321-323.
[5]Yu Y,Wei H Z,Yu L,et al.Catalytic wet air oxidation of m-cresol over a surface-modified sewage sludge-derived carbonaceous catalyst[J].Catalysis Science&Technology,2016,6(4):1085-1093.
[6]Yu Y,Wei H Z,Yu L,et al.Sewage-sludge-derived carbonaceous materials for catalytic wet hydrogen peroxide oxidation of m-cresol in batch and continuous reactors[J].Environmental Technology,2016,37(2):153-162.
[7]Zhou H,Guo J J,Li P,et al.Leaf-architectured 3D hierarchical artificial photosynthetic system of perovskite titanates towards CO2photoreduction into hydrocarbon fuels[J].Scientific Reports,2013,3.
[8]张小玲,班云霄.LED联合玻璃纤维光催化填料对苯酚的降解研究[J].中国环境科学,2018,38(8):2941-2946.Zhang X L,Ban Y X.Study on the degradation of phenol by UV-LEDcombined with glass fiber photocatalytic fillers[J].China Environmental Science,2018,38(8):2941-2946.
[9]Sires I,Brillas E,Oturan M A,et al.Electrochemical advanced oxidation processes:today and tomorrow.A review[J].Environmental Science and Pollution Research,2014,21(14):8336-8367.
[10]Hermosilla D,Merayo N,Gasco A,et al.The application of advanced oxidation technologies to the treatment of effluents from the pulp and paper industry:a review[J].Environmental Science and Pollution Research,2015,22(1):168-191.
[11]Xiong Y,He C,Karlsson H T,et al.Performance of three-phase three-dimensional electrode reactor for the reduction of COD in simulated wastewater-containing phenol[J].Chemosphere,2003,50(1):131-136.
[12]Xiong Y,He C,An T C,et al.Removal of formic acid from wastewater using three-phase three-dimensional electrode reactor[J].Water,Air,and Soil Pollution,2003,144(1):67-79.
[13]伍波,李鹏,张波,等.负载型粒子电极电催化氧化苯酚的研究[J].中国环境科学,2015,35(8):2426-2432.Wu B,Li P,Zhang B,et al.Electro-catalytic performance of the activated carbon supported metal oxide as particulate electrode for phenol oxidation[J].China Environmental Science,2015,35(8):2426-2432.
[14]Wu X B,Yang X Q,Wu D C,et al.Feasibility stud of using carbon aerogel as particle electrodes for decoloration of RBRX dye solution in a three-dimensional electrode reactor[J].Chemical Engineering Journal,2008,138(1-3):47-54.
[15]Boudenne J L,Cerclier O.Performance of carbon black-slurry electrodes for 4-chlorophenol oxidation[J].Water Research,1999,33(2):494-504.
[16]Sharifian H,Kirk D W.Electrochemical oxidation of phenol[J].Journal of the Electrochemical Society,1986,133(5):921-924.
[17]张芳,李光明,盛怡,等.电催化氧化法处理苯酚废水的Mn-SnSb/γ-Al2O3粒子电极研制[J].化学学报,2006,64(3):235-239.Zhang F,Li G M,Sheng Y,et al.Preparation of Mn-Sn-Sb/γ-Al2O3particle-electrodes for electrocatalytic oxidation of phenol wastewater[J].Acta Chimica Sinica,2006,64(3):235-239.
[18]Gu L,Wang B,Ma H Z,et al.Catalytic oxidation of anionic surfactants by electrochemical oxidation with Cu O-Co2O3-PO43-modified kaolin[J].Journal of Hazardous Materials,2006,137(2):842-848.
[19]Ma L,Sun C L,Ren J,et al.Efficient electrochemical incineration of phenol on activated carbon fiber as a new type of particulates[J].Russian Journal of Electrochemistry,2014,50(6):569-578.
[20]Chou W L,Wang C T,Chang C P.Comparison of removal of Acid Orange 7 by electrooxidation using various anode materials[J].Desalination,2011,266(1-3):201-207.
[21]Hueso J L,Espinós J P,Caballero A,et al.XPS investigation of the reaction of carbon with NO,O2,N2 and H2O plasmas[J].Carbon,2007,45(1):89-96.
[22]孙杰,钟超,彭巧丽.活性炭纤维复合阴极材料电芬顿降解苯酚[J].中南民族大学学报(自然科学版),2015,34(2):6.Sun J,Zhong C,Peng Q L.Electro-Fenton degradation of phenol using hybridized activated carbon fiber as cathode materials[J].Journal of SouthCentral University for Nationalities(Natural Science Edition),2015,34(2):6.