銅納米柱修飾錫銻電極的制備及其在耦合過程中的應用
發(fā)布時間：2018-10-08 20:09
【摘要】：鈦基氧化錫銻電極Ti/SnO2-Sb是電催化氧化法水處理工藝中較為有效的電極體系,但普遍存在能耗較高、導電性不夠理想、電極穩(wěn)定性較弱等不足,催化活性也有待進一步提升。本文首次使用高度線性有序的銅納米柱陣列對基體進行微觀結(jié)構(gòu)設計,由AAO模板輔助電沉積法制備出具有大比表面積、高催化活性與穩(wěn)定性、低電荷傳遞阻力的銅納米柱修飾鈦基錫銻電極Ti/CuNRs/SnO2-Sb,并將其應用于電催化氧化與納濾的耦合過程中,研究電極體系差異對耦合過程水處理性能的影響。本文首先對Ti/SnO2-Sb電極與Ti/Cu-NRs/SnO2-Sb電極進行物理表征,SEM對比研究結(jié)果表明,銅納米柱均勻的分布在基體表面,直徑為200-300nm,長度約2um。Ti/Cu-NRs/SnO2-Sb電極催化層形貌更為均勻致密,結(jié)構(gòu)缺陷較少。經(jīng)XRD測試,基體表面覆蓋良好,銅柱使得催化層的晶胞參數(shù)明顯減小。這種高度有序的一維納米結(jié)構(gòu)所形成的三維空間,能夠為催化劑提供較大的負載空間和充足的溶質(zhì)分子吸附位點與反應位點。Ti/Cu-NRs/SnO2-Sb電極具有較高的析氧電位,為2.17V。銅納米柱結(jié)構(gòu)的存在使得Ti/Cu-NRs/SnO2-Sb電極的比表面積大幅提高,伏安電荷量為傳統(tǒng)電極1.8倍。銅柱在SnO2-Sb催化層中起著類似導線的作用,明顯改善電極體系的電荷傳遞路徑與阻力,EIS測試結(jié)果證實,Ti/Cu-NRs/SnO2-Sb電極的電化學阻抗僅為Ti/SnO2-Sb電極的15.4%。銅柱的存在同樣使得電極穩(wěn)定性有了較大提升,強化壽命測試結(jié)果表明,Ti/Cu-NRs/SnO2-Sb電極的強化壽命為Ti/SnO2-Sb電有的1.6倍。AR73染料廢水的催化降解過程中,采用Ti/Cu-NRs/SnO2-Sb電極的色度去除率比Ti/SnO2-Sb電極高出10%。銅柱使得電極體系的整體電荷傳遞阻力減小,降解過程槽電壓下降0.7V,AR73降解80%時,能耗下降24.5%。電催化降解能耗的降低,使得Ti/Cu-NRs/SnO2-Sb電極在水處理工藝中的經(jīng)濟合理性增強。Ti/Cu-NRs/SnO2-Sb電極首次被引入到電催化氧化與納濾的耦合過程中,與Ti/SnO2-Sb電極相比,新型電極的使用使得滲透通量也有較大提高。
[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.
【學位授予單位】：天津大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：X703;O646
本文編號：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.
【學位授予單位】：天津大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：X703;O646
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