高效能活性炭基底石墨烯粒子电极制备及表征
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摘要
目的制备和筛选出一种高效、稳定的新型石墨烯复合负载型粒子电极.方法采用溶胶凝胶法制备了一系列不同基底的石墨烯负载型粒子电极,以苯酚为目标污染物考察粒子电极的催化活性,确定最优粒子电极,通过正交试验优化其制备条件.最后采用SEM、EDS、BET、XRD、LSV、CV手段对粒子电极的结构、表面形貌及电化学性能等进行表征.结果筛选出Ti-r GO/GAC-S(椰壳活性炭)为最优粒子电极,对苯酚去除率为85. 26%;正交试验优化其制备条件为钛酸丁酯投加量75 mL、r GO投加量0. 2 g、煅烧温度400℃、煅烧时间1 h;负载Ti和r GO后表面积、析氧电位增大,对苯酚直接氧化能力提高.结论筛选出的Ti-r GO/GAC-S粒子电极电催化活性最高,表面积大,活性点位多,对苯酚的直接氧化能力高.
To prepare and screen a newtype of graphene composite supported particle electrode with high efficiency and stability. A series of graphene-loaded particle electrodes with different substrates were prepared by sol-gel method. The catalytic activity of the particle electrode was investigated with phenol as the target contaminant. The optimal particle electrode was determined and the preparation conditions were optimized by orthogonal test. Finally,SEM,EDS,BET,XRD,LSV,and CV methods were used to characterize the structure,surface morphology and electrochemical properties of the particle electrode. The results showed that Ti-rGO/GAC-S( coconic activated carbon) was selected as the best particle electrode,and the removal rate of phenol was85. 26%. Orthogonal experiments optimize the preparation conditions as follows: the dosage of butyl titanate is 75 mL,the dosage of r GO is 0. 2 g,the calcination temperature is 400 ℃,the calcination time is 1 h; surface area and oxygen evolution potential increase after loading Ti and r GO,and the direct oxidation ability of phenol is improved. The conclusion is that the selected Ti-rGO/GAC-S particle electrode has the highest electrocatalytic activity,large surface area,many active sites,and high direct oxidation ability to phenol.
To prepare and screen a newtype of graphene composite supported particle electrode with high efficiency and stability. A series of graphene-loaded particle electrodes with different substrates were prepared by sol-gel method. The catalytic activity of the particle electrode was investigated with phenol as the target contaminant. The optimal particle electrode was determined and the preparation conditions were optimized by orthogonal test. Finally,SEM,EDS,BET,XRD,LSV,and CV methods were used to characterize the structure,surface morphology and electrochemical properties of the particle electrode. The results showed that Ti-rGO/GAC-S( coconic activated carbon) was selected as the best particle electrode,and the removal rate of phenol was85. 26%. Orthogonal experiments optimize the preparation conditions as follows: the dosage of butyl titanate is 75 mL,the dosage of r GO is 0. 2 g,the calcination temperature is 400 ℃,the calcination time is 1 h; surface area and oxygen evolution potential increase after loading Ti and r GO,and the direct oxidation ability of phenol is improved. The conclusion is that the selected Ti-rGO/GAC-S particle electrode has the highest electrocatalytic activity,large surface area,many active sites,and high direct oxidation ability to phenol.
引文
[1] KUMAR S,OJHA A K,PATRICE D,et al.One-step in situ synthesis of CeO2nano particles grown on reduced graphene oxide as an excellent fluorescent and photocatalyst material under sunlight irradiation[J]. Physical chemistry chemical physics,2016,18(16):11157-11167.
[2] KUMAR D R,WANGYan,VASILYEVA S V,et al. Extraordinary hydrogen evolution and oxidation reaction activity from carbon nano tubes and graphitic carbons[J]. Acsnano,2014,8(8):8447-8456.
[3]唐朝春,段先月,叶鑫,等.石墨烯的制备及其在水处理中的应用研究进展[J].工业水处理,2017,37(3):10-15.(TANGChaochun,Duan Xianyue,Ye Xin,et al. Progress in the preparation of graphene and its application to water treatment[J]. Industrial water treatment,2017,37(3):10-15.)
[4]吴诗德,宋彦良,李超,等.石墨烯材料的制备及其在电化学领域的应用[J].材料导报,2011,25(3):55-59.(WU Shide,SONGYanliang,LI Chao,et al.Preparation and applications in electrochemistry of graphene-based materials[J]. Materials review,2011,25(3):55-59.)
[5]傅金祥,孟海停,何祥,等.石墨烯及其复合材料在环境领域中的应用研究进展[J].环境污染与防治,2018,40(5):609-615.(FU Jinxiang,MENGHaiting,HE Xiang,et al. Research progress on enviromental applications of graphene and its composites[J]. Environmental pollution and control,2018,40(5):609-615.)
[6]班福忱,赵晓彤,武玉萍,等.三维电极/电Fenton法处理苯酚废水机理研究[J].沈阳建筑大学学报(自然科学版),2014,30(1):137-141.(BAN Fuchen,ZHAO Xiaotong,WU Yuping,et al. Study on mechanism of phenol wastewater degradation by three-dimensional/electrical-fenton method[J]. Journal of Shenyang jianzhu university(natural science),2014,30(1):137-141.)
[7] ZHAO X,LI A,MAO R,et al. Electrochemical removal of haloacetic acids in a three-dimensional electrochemical reactor with Pd-GAC particles as fixed filler and Pd-modified carbon paper as cathode[J]. Water research,2014,51(1):134.
[8]张显峰,王德军,赵朝成,等.三维电极电催化氧化法处理废水的研究进展[J].物理化学学报,2016,36(3):250-254.(ZHANGXianfeng,WANGDejun,ZHAO Chaocheng,et al. Research progress in treatment of wastewater by three-dimensional electrode catalytic oxidation process[J]. Acta phys. sinica,2016,36(3):250-254.)
[9] HE Wenyan,MA Qingliang,WANGJing,et al. Preparation of novel kaolin-based particle electrodes for treating methyl orange wastewater[J]. Applied clay science,2014,99:178-186.
[10] CHEN Z,ZHANGY,ZHOU L,et al. Performance of nitrogen-doped graphene aerogel particle electrodes for electro-catalytic oxidation of simulated bisphenol a wastewaters[J]. Journal of hazardous materials,2017,332:70-78.
[11]吴娜娜,郑璐,李亚峰,等.三维电极法处理有机废水的研究进展[J].工业水处理,2016,36(8):840-846.(WU Nana,ZHENGLu,LI Yafeng,et al. Research progress in the treatment of organic wastewater by three-dimensional electrode method[J]. Industrial water treatment,2016,36(8):840-846.)
[12]刘文卿.实验设计[M].北京:清华大学出版社,2002.(LIU Wenqing. Experimental design[M].Beijing:Tsinghua university press,2002.)
[13]辛岳红,魏刚,魏云鹏,等.沸石负载复合氧化物粒子电极的制备及其电催化活性[J].北京化工大学学报(自然科学版),2010,37(2):54-58.(XIN Yuehong,WEI Gang,WEI Yunpeng,et al. Preparation of particle electrodes of zeolites loaded with composite oxides and a study of their electrocatalytic activity[J]. Journal of Beijing university of chemical technology(natural science edition),2010,37(2):54-58.)
[14] LI X Y,CUI Y H,FENGY J,et al. Reaction pathways and mechanisms of the electrochemical degradation of phenol on different electrodes[J]. Water research,2005,39(10):1972-81.
[15]查全性.电极过程动力学导论[M]. 3版.北京:科学出版社,2002.(CHA Quanxing. Introduction to electrode process dynamics[M]. 3rd ed. Beijing:Science Press,2002.)
[16] LIU Wei,AI Zhihui,ZHANGLizhi. Design of a neutral three-dimensional electro-fenton system with foamnickel as particle electrodes for wastewater treatment[J]. Journal of hazardous materials,2012,243:257-264.
[17] MOHAJERI S,AZIZ H A,ISA MH,et al.Statistical optimization of process parameters for landfill leachate treatment using electro-fenton technique[J]. Journal of hazardous materials,2010,176(1/2/3):749-758.
[18] NIDHEESH P V,GANDHIMATHIR. Trends in electro-fenton process for water and wastewater treatment:An overview[J]. Desalination,2012,299:1-15.
[2] KUMAR D R,WANGYan,VASILYEVA S V,et al. Extraordinary hydrogen evolution and oxidation reaction activity from carbon nano tubes and graphitic carbons[J]. Acsnano,2014,8(8):8447-8456.
[3]唐朝春,段先月,叶鑫,等.石墨烯的制备及其在水处理中的应用研究进展[J].工业水处理,2017,37(3):10-15.(TANGChaochun,Duan Xianyue,Ye Xin,et al. Progress in the preparation of graphene and its application to water treatment[J]. Industrial water treatment,2017,37(3):10-15.)
[4]吴诗德,宋彦良,李超,等.石墨烯材料的制备及其在电化学领域的应用[J].材料导报,2011,25(3):55-59.(WU Shide,SONGYanliang,LI Chao,et al.Preparation and applications in electrochemistry of graphene-based materials[J]. Materials review,2011,25(3):55-59.)
[5]傅金祥,孟海停,何祥,等.石墨烯及其复合材料在环境领域中的应用研究进展[J].环境污染与防治,2018,40(5):609-615.(FU Jinxiang,MENGHaiting,HE Xiang,et al. Research progress on enviromental applications of graphene and its composites[J]. Environmental pollution and control,2018,40(5):609-615.)
[6]班福忱,赵晓彤,武玉萍,等.三维电极/电Fenton法处理苯酚废水机理研究[J].沈阳建筑大学学报(自然科学版),2014,30(1):137-141.(BAN Fuchen,ZHAO Xiaotong,WU Yuping,et al. Study on mechanism of phenol wastewater degradation by three-dimensional/electrical-fenton method[J]. Journal of Shenyang jianzhu university(natural science),2014,30(1):137-141.)
[7] ZHAO X,LI A,MAO R,et al. Electrochemical removal of haloacetic acids in a three-dimensional electrochemical reactor with Pd-GAC particles as fixed filler and Pd-modified carbon paper as cathode[J]. Water research,2014,51(1):134.
[8]张显峰,王德军,赵朝成,等.三维电极电催化氧化法处理废水的研究进展[J].物理化学学报,2016,36(3):250-254.(ZHANGXianfeng,WANGDejun,ZHAO Chaocheng,et al. Research progress in treatment of wastewater by three-dimensional electrode catalytic oxidation process[J]. Acta phys. sinica,2016,36(3):250-254.)
[9] HE Wenyan,MA Qingliang,WANGJing,et al. Preparation of novel kaolin-based particle electrodes for treating methyl orange wastewater[J]. Applied clay science,2014,99:178-186.
[10] CHEN Z,ZHANGY,ZHOU L,et al. Performance of nitrogen-doped graphene aerogel particle electrodes for electro-catalytic oxidation of simulated bisphenol a wastewaters[J]. Journal of hazardous materials,2017,332:70-78.
[11]吴娜娜,郑璐,李亚峰,等.三维电极法处理有机废水的研究进展[J].工业水处理,2016,36(8):840-846.(WU Nana,ZHENGLu,LI Yafeng,et al. Research progress in the treatment of organic wastewater by three-dimensional electrode method[J]. Industrial water treatment,2016,36(8):840-846.)
[12]刘文卿.实验设计[M].北京:清华大学出版社,2002.(LIU Wenqing. Experimental design[M].Beijing:Tsinghua university press,2002.)
[13]辛岳红,魏刚,魏云鹏,等.沸石负载复合氧化物粒子电极的制备及其电催化活性[J].北京化工大学学报(自然科学版),2010,37(2):54-58.(XIN Yuehong,WEI Gang,WEI Yunpeng,et al. Preparation of particle electrodes of zeolites loaded with composite oxides and a study of their electrocatalytic activity[J]. Journal of Beijing university of chemical technology(natural science edition),2010,37(2):54-58.)
[14] LI X Y,CUI Y H,FENGY J,et al. Reaction pathways and mechanisms of the electrochemical degradation of phenol on different electrodes[J]. Water research,2005,39(10):1972-81.
[15]查全性.电极过程动力学导论[M]. 3版.北京:科学出版社,2002.(CHA Quanxing. Introduction to electrode process dynamics[M]. 3rd ed. Beijing:Science Press,2002.)
[16] LIU Wei,AI Zhihui,ZHANGLizhi. Design of a neutral three-dimensional electro-fenton system with foamnickel as particle electrodes for wastewater treatment[J]. Journal of hazardous materials,2012,243:257-264.
[17] MOHAJERI S,AZIZ H A,ISA MH,et al.Statistical optimization of process parameters for landfill leachate treatment using electro-fenton technique[J]. Journal of hazardous materials,2010,176(1/2/3):749-758.
[18] NIDHEESH P V,GANDHIMATHIR. Trends in electro-fenton process for water and wastewater treatment:An overview[J]. Desalination,2012,299:1-15.
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