铝掺杂改性钛基PbO_2电极性能研究
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摘要
采用阳极电沉积技术制备了金属铝掺杂改性的钛基PbO_2电极。通过表面粗糙度测量,扫描电镜、X射线衍射结构分析,线性极化和交流阻抗谱电化学测试和加速寿命试验分析了铝掺杂对PbO_2涂层电极的物理化学特性的影响并考察了铝掺杂PbO_2电极对苯酚模拟废水的电催化氧化降解行为。结果表明,Al~(3+)添加可使得PbO_2电极涂层结晶细化、沉积均匀致密,表面粗糙度明显降低,结瘤缺陷改善;铝掺杂改性的PbO_2电极析氧电位升高,电荷传递及催化性能提高,但呈非单调变化,其中添加3 mmol/L Al~(3+)制备电极的析氧电位最高,可达2.09 V,导电性优异,电催化性能最佳,电化学稳定性高,其强化寿命可达460 h,比未掺杂电极寿命提高了100 h。铝掺杂改性的PbO_2电极对苯酚模拟废水具有良好的降解能力,180 min处理后苯酚去除率最高可达94%,COD去除率最大可达73.6%。
Al-doped Ti/PbO_2 electrodes were prepared by anodic deposition from solution containing Al(III)cation.Influence of Al-doping on the physicochemical properties of modified PbO_2 coating electrodes was characterized by surface roughometer,scanning electron microscope(SEM),X-ray diffraction(XRD),linear polarization and electrochemical impedance spectroscopy(EIS)techniques,and accelerated life test.The electrocatalytic oxidation degradation behavior of Al-doping PbO_(2 )electrodes for phenol simulation wastewater was compared.The results show that PbO_(2 )coatings with smaller grain size,uniform and dense surface,lower surface roughness and less nodulation defect are obtained when a certain amount of Al~(3+)is added into the electrodeposition solution.Al-doping results in the increase of oxygen evolution potential,improvement of charge transfer capacity and enhancement of electrocatalytic performance for PbO_2electrodes.Nevertheless,these properties do not uniformly vary with increase of Al~(3+)addition amount.When deposited for 3 h in the bath solution containing 3 mmol/L Al~(3+),the prepared electrode has maximum oxygen evolution potential 2.09 V,excellent electrical conductivity,the best electrocatalytic property and the longest accelerated life of 460 h.The Al-doped Ti/PbO_2 electrodes show excellent electrochemical oxidation degradation capacity for phenol simulated wastewater.After treatment for 180 min the removal rate of phenol is up to 94%,and the maximum removal rate of COD can reach 73.6%.
Al-doped Ti/PbO_2 electrodes were prepared by anodic deposition from solution containing Al(III)cation.Influence of Al-doping on the physicochemical properties of modified PbO_2 coating electrodes was characterized by surface roughometer,scanning electron microscope(SEM),X-ray diffraction(XRD),linear polarization and electrochemical impedance spectroscopy(EIS)techniques,and accelerated life test.The electrocatalytic oxidation degradation behavior of Al-doping PbO_(2 )electrodes for phenol simulation wastewater was compared.The results show that PbO_(2 )coatings with smaller grain size,uniform and dense surface,lower surface roughness and less nodulation defect are obtained when a certain amount of Al~(3+)is added into the electrodeposition solution.Al-doping results in the increase of oxygen evolution potential,improvement of charge transfer capacity and enhancement of electrocatalytic performance for PbO_2electrodes.Nevertheless,these properties do not uniformly vary with increase of Al~(3+)addition amount.When deposited for 3 h in the bath solution containing 3 mmol/L Al~(3+),the prepared electrode has maximum oxygen evolution potential 2.09 V,excellent electrical conductivity,the best electrocatalytic property and the longest accelerated life of 460 h.The Al-doped Ti/PbO_2 electrodes show excellent electrochemical oxidation degradation capacity for phenol simulated wastewater.After treatment for 180 min the removal rate of phenol is up to 94%,and the maximum removal rate of COD can reach 73.6%.
引文
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[2]Li Xiaoliang,Xu Hao,Yan Wei et al.Journal of Alloys and Compounds[J],2017,718:386
[3]Khum Gurung,Mohamed Chaker Ncibi,Marina Shestakova et al.Applied Catalysis B:Environmental[J],2018,221:329
[4]Aleix Benito,Aida Penadés,Josep Lluis Lliberia et al.Chemosphere[J],2017,166:230
[5]Xu Pindi(徐品弟),Liu Houtian(柳厚田).Battery(蓄电池)[J],1994(2):1
[6]Dai Qizhou,Xia Yijing,Chen Jianmeng et al.Electrochimica Acta[J],2016,188:871
[7]Xu Hao,Li Jingjing,Yan Wei et al.Rare Metal Materials and Engineering[J],2013,42(5):885
[8]Chen Jianmeng,Xia Yijing,Dai Qizhou et al.Electrochimica Acta[J],2015,165:277
[9]Xia Yijing,Dai Qizhou,Chen Jianmeng et al.Journal of Electroanalytical Chemistry[J],2015,744:117
[10]Shmychkova O,Luk’yanenko T,Velichenko A et al.Electrochimica Acta[J],2013,111:332
[11]Dai Qizhou,Zhou Jiazhong,Meng Xiaoyang et al.Chemical Engineering Journal[J],2016,289:239
[12]Wang Lei(王磊),Xue Juanqin(薛娟琴),Yu Lihua(于丽花)et al.Electrochemical(电化学)[J],2017,23(4):480
[13]Yu Lihua,Xue Juanqin,Wang Lei et al.Rare Metal Materials and Engineering[J],2017,46(7):1833
[14]Velichenko A B,Devilliers D.Journal of Fluorine Chemistry[J],2007,128(4):269
[15]Duan Xiaoyue,Zhao Cuimei,Liu Wei et al.Electrochimica Acta[J],2017,240:424
[16]Hu J M,Meng H M,Zhang J Q et al.Corrosion Science[J],2002,44(8):1655
[17]Zhao Wei,Xing Juntao,Chen Donghui et al.RSC Advances[J],2015,5(34):26 530
[18]Yang Kun,Liu Yuyu,Qiao Jinli et al.Separation and Purification Technology[J],2017,189:459
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