铜纳米柱修饰锡锑电极的制备及其在耦合过程中的应用
发布时间：2018-10-08 20:09
【摘要】：钛基氧化锡锑电极Ti/SnO2-Sb是电催化氧化法水处理工艺中较为有效的电极体系,但普遍存在能耗较高、导电性不够理想、电极稳定性较弱等不足,催化活性也有待进一步提升。本文首次使用高度线性有序的铜纳米柱阵列对基体进行微观结构设计,由AAO模板辅助电沉积法制备出具有大比表面积、高催化活性与稳定性、低电荷传递阻力的铜纳米柱修饰钛基锡锑电极Ti/CuNRs/SnO2-Sb,并将其应用于电催化氧化与纳滤的耦合过程中,研究电极体系差异对耦合过程水处理性能的影响。本文首先对Ti/SnO2-Sb电极与Ti/Cu-NRs/SnO2-Sb电极进行物理表征,SEM对比研究结果表明,铜纳米柱均匀的分布在基体表面,直径为200-300nm,长度约2um。Ti/Cu-NRs/SnO2-Sb电极催化层形貌更为均匀致密,结构缺陷较少。经XRD测试,基体表面覆盖良好,铜柱使得催化层的晶胞参数明显减小。这种高度有序的一维纳米结构所形成的三维空间,能够为催化剂提供较大的负载空间和充足的溶质分子吸附位点与反应位点。Ti/Cu-NRs/SnO2-Sb电极具有较高的析氧电位,为2.17V。铜纳米柱结构的存在使得Ti/Cu-NRs/SnO2-Sb电极的比表面积大幅提高,伏安电荷量为传统电极1.8倍。铜柱在SnO2-Sb催化层中起着类似导线的作用,明显改善电极体系的电荷传递路径与阻力,EIS测试结果证实,Ti/Cu-NRs/SnO2-Sb电极的电化学阻抗仅为Ti/SnO2-Sb电极的15.4%。铜柱的存在同样使得电极稳定性有了较大提升,强化寿命测试结果表明,Ti/Cu-NRs/SnO2-Sb电极的强化寿命为Ti/SnO2-Sb电有的1.6倍。AR73染料废水的催化降解过程中,采用Ti/Cu-NRs/SnO2-Sb电极的色度去除率比Ti/SnO2-Sb电极高出10%。铜柱使得电极体系的整体电荷传递阻力减小,降解过程槽电压下降0.7V,AR73降解80%时,能耗下降24.5%。电催化降解能耗的降低,使得Ti/Cu-NRs/SnO2-Sb电极在水处理工艺中的经济合理性增强。Ti/Cu-NRs/SnO2-Sb电极首次被引入到电催化氧化与纳滤的耦合过程中,与Ti/SnO2-Sb电极相比,新型电极的使用使得渗透通量也有较大提高。
[Abstract]:Titanium based tin antimony oxide electrode Ti/SnO2-Sb is a more effective electrode system in the electrocatalytic oxidation process, but there are many disadvantages such as high energy consumption, low conductivity, weak electrode stability and so on, and the catalytic activity needs to be further improved. In this paper, a highly linear and ordered copper nanocolumn array is used to design the microstructure of the matrix for the first time. Large specific surface area, high catalytic activity and stability have been prepared by AAO template assisted electrodeposition method. Low charge transfer resistance copper nano-column modified titanium-based tin antimony electrode Ti/CuNRs/SnO2-Sb, was applied to the coupling process of electrocatalytic oxidation and nanofiltration. The effect of electrode system difference on the water treatment performance in the coupling process was studied. In this paper, the physical characterizations of Ti/SnO2-Sb electrode and Ti/Cu-NRs/SnO2-Sb electrode were compared. The results showed that the copper nanocolumn was uniformly distributed on the surface of the substrate, with a diameter of 200-300 nm, and the catalytic layer was more uniform and compact in length than that of the 2um.Ti/Cu-NRs/SnO2-Sb electrode, and the structure defects were less. The results of XRD show that the substrate surface is well covered and the cell parameters of the catalyst layer are obviously reduced by copper column. The three-dimensional space formed by this highly ordered one-dimensional nanostructure can provide the catalyst with a large loading space and sufficient solute molecular adsorption sites and reaction sites. TirCu-NRsr / SnO2-Sb electrode has a higher oxygen evolution potential (2.17V). The specific surface area of Ti/Cu-NRs/SnO2-Sb electrode was greatly increased by the presence of copper nanocolumn structure, and the voltammetric charge was 1.8 times higher than that of conventional electrode. Copper column acts as a traverse in the SnO2-Sb catalytic layer. It is proved that the electrochemical impedance of TiR / Cu-NRsR / SnO2-Sb electrode is only 15.4% of that of Ti/SnO2-Sb electrode, which improves the charge transfer path and resistance of the electrode system. The existence of copper column also improved the stability of the electrode. The test results of strengthening life showed that the enhanced lifetime of Ti / Cu-NRs / SnO2-Sb electrode was 1.6 times that of Ti/SnO2-Sb. AR73 dye wastewater was degraded in the process of catalytic degradation. The chromaticity removal rate of Ti/Cu-NRs/SnO2-Sb electrode is 10% higher than that of Ti/SnO2-Sb electrode. The overall charge transfer resistance of the electrode system was reduced by copper column, and the cell voltage decreased by 0.7V AR73, and the energy consumption decreased by 24.5. With the reduction of energy consumption of electrocatalytic degradation, the economic reasonableness of Ti/Cu-NRs/SnO2-Sb electrode in water treatment process is enhanced. The Ti- / Cu-NRs-SnO2-Sb electrode is introduced into the coupling process of electrocatalytic oxidation and nanofiltration for the first time, compared with Ti/SnO2-Sb electrode. With the use of new electrodes, the permeation flux is also greatly improved.
【学位授予单位】：天津大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：X703;O646
本文编号：2258105
[Abstract]:Titanium based tin antimony oxide electrode Ti/SnO2-Sb is a more effective electrode system in the electrocatalytic oxidation process, but there are many disadvantages such as high energy consumption, low conductivity, weak electrode stability and so on, and the catalytic activity needs to be further improved. In this paper, a highly linear and ordered copper nanocolumn array is used to design the microstructure of the matrix for the first time. Large specific surface area, high catalytic activity and stability have been prepared by AAO template assisted electrodeposition method. Low charge transfer resistance copper nano-column modified titanium-based tin antimony electrode Ti/CuNRs/SnO2-Sb, was applied to the coupling process of electrocatalytic oxidation and nanofiltration. The effect of electrode system difference on the water treatment performance in the coupling process was studied. In this paper, the physical characterizations of Ti/SnO2-Sb electrode and Ti/Cu-NRs/SnO2-Sb electrode were compared. The results showed that the copper nanocolumn was uniformly distributed on the surface of the substrate, with a diameter of 200-300 nm, and the catalytic layer was more uniform and compact in length than that of the 2um.Ti/Cu-NRs/SnO2-Sb electrode, and the structure defects were less. The results of XRD show that the substrate surface is well covered and the cell parameters of the catalyst layer are obviously reduced by copper column. The three-dimensional space formed by this highly ordered one-dimensional nanostructure can provide the catalyst with a large loading space and sufficient solute molecular adsorption sites and reaction sites. TirCu-NRsr / SnO2-Sb electrode has a higher oxygen evolution potential (2.17V). The specific surface area of Ti/Cu-NRs/SnO2-Sb electrode was greatly increased by the presence of copper nanocolumn structure, and the voltammetric charge was 1.8 times higher than that of conventional electrode. Copper column acts as a traverse in the SnO2-Sb catalytic layer. It is proved that the electrochemical impedance of TiR / Cu-NRsR / SnO2-Sb electrode is only 15.4% of that of Ti/SnO2-Sb electrode, which improves the charge transfer path and resistance of the electrode system. The existence of copper column also improved the stability of the electrode. The test results of strengthening life showed that the enhanced lifetime of Ti / Cu-NRs / SnO2-Sb electrode was 1.6 times that of Ti/SnO2-Sb. AR73 dye wastewater was degraded in the process of catalytic degradation. The chromaticity removal rate of Ti/Cu-NRs/SnO2-Sb electrode is 10% higher than that of Ti/SnO2-Sb electrode. The overall charge transfer resistance of the electrode system was reduced by copper column, and the cell voltage decreased by 0.7V AR73, and the energy consumption decreased by 24.5. With the reduction of energy consumption of electrocatalytic degradation, the economic reasonableness of Ti/Cu-NRs/SnO2-Sb electrode in water treatment process is enhanced. The Ti- / Cu-NRs-SnO2-Sb electrode is introduced into the coupling process of electrocatalytic oxidation and nanofiltration for the first time, compared with Ti/SnO2-Sb electrode. With the use of new electrodes, the permeation flux is also greatly improved.
【学位授予单位】：天津大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：X703;O646
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