多孔鈦基摻銻二氧化錫管式膜電極的制備及其催化性能研究
發(fā)布時間：2018-10-30 12:11
【摘要】：電催化氧化技術(shù)以其環(huán)境兼容性和環(huán)境友好性等特點引起環(huán)境學(xué)界廣泛關(guān)注。開發(fā)電催化活性高、使用壽命長的高性能陽極材料是學(xué)者研究的熱點。本文從制備方法和改變基體材料結(jié)構(gòu)兩個方面入手,旨在設(shè)計出合理的反應(yīng)器、制備出一種兼具電催化活性和膜過濾性能的多孔Ti/Sb-SnO2管式膜電極,以期提高電極性能和電荷利用率,從而能夠高效地催化降解水中污染物。以鈦濾管代替?zhèn)鹘y(tǒng)鈦板為基體,采用不同的制備方法得到了具有不同表面微觀結(jié)構(gòu)的多孔Ti/Sb-SnO2管式膜電極。SEM、孔徑分布測試技術(shù)表征結(jié)果顯示,采用Pechini法和超聲浸沒法結(jié)合制備所得的電極晶粒尺寸較小,通過多次超聲浸沒熱分解過程可以顯著改善多孔電極內(nèi)部的孔徑分布,平均孔徑從2.607μm減小為2.278μm,具有較大的電化學(xué)活性表面。LSV測試表明,采用Pechini法和超聲浸沒法結(jié)合制備所得的管狀多孔Ti/Sb-SnO2電極在酸性、中性、堿性三種介質(zhì)中的析氧電位分別為2.02V、2.01V、1.10V。溶液的pH值對電極的析氧電位影響較大,在堿性條件下的析氧電位明顯劣于酸性條件。而溶膠凝膠法制備所得電極在0.5 mol/L Na2SO4溶液中析氧電位僅為1.44V。為探究制備電極是否具有電催化氧化和膜過濾協(xié)同作用,應(yīng)用同一電極在相同電解條件下分別在普通裝置和工藝組合裝置中處理初始濃度為100mg/L的吡啶模擬廢水,結(jié)果表明它們對毗啶去除率分別是51.96%和69.89%,通過計算電流瞬時效率,后者的電荷利用率高�？疾炝瞬煌跏歼拎舛�、電解質(zhì)濃度、電流密度、初始pH值對吡啶去除效果的影響來探究制備電極電催化性能。在電解質(zhì)濃度(無水硫酸鈉)10.0 g/L、電流密度30 mA/cm2、pH=3的最優(yōu)參數(shù)條件,100mg/L吡啶廢水降解處理180min的去除率達(dá)100%。從UV、HPLC和IC來分析水樣得出,管式多孔Ti/Sb-SnO2陽極電催化氧化降解吡啶的過程對其中間產(chǎn)物也有催化氧化效果,降解過程中會產(chǎn)生甲酸和乙酸這種小分子有機酸,還檢測到有硝酸根離子和亞硝酸根離子生成�？梢酝茰y吡啶是在管式多孔Ti/Sb-SnO2陽極表面斷了C-N鍵使得吡啶開環(huán)然后利于后續(xù)降解效果。
[Abstract]:Electrocatalytic oxidation (EO) technology has attracted wide attention in the field of environment because of its environmental compatibility and environmental friendliness. The development of high performance anode materials with high electrocatalytic activity and long service life is a hot research topic. The purpose of this paper is to design a reasonable reactor to prepare a porous Ti/Sb-SnO2 tubular membrane electrode with both electrocatalytic activity and membrane filtration performance. In order to improve the electrode performance and charge utilization, it can efficiently catalyze the degradation of pollutants in water. Porous Ti/Sb-SnO2 tubular membrane electrode with different surface microstructure was obtained by using titanium filter tube instead of traditional titanium plate as substrate. The SEM, pore size distribution was characterized by SEM, pore size distribution technique. The grain size of the electrode which could not be prepared by Pechini method and ultrasonic immersion was small. The pore size distribution in porous electrode could be significantly improved by multiple ultrasonic immersion thermal decomposition process, and the average pore size was reduced from 2.607 渭 m to 2.278 渭 m. The results of LSV test showed that the oxygen evolution potential of tubular porous Ti/Sb-SnO2 electrode in acidic, neutral and alkaline media was 2.02V ~ (2.01V), respectively, which could not be prepared by Pechini and ultrasonic immersion, and the results showed that the oxygen evolution potential of tubular porous Ti/Sb-SnO2 electrode was 2.02V ~ (-1) V in acidic, neutral and alkaline media. 1.10V. The pH value of the solution has a great influence on the oxygen evolution potential of the electrode, and the oxygen evolution potential in the alkaline condition is obviously inferior to that in the acidic condition. However, the oxygen evolution potential of the electrode prepared by sol-gel method is only 1.44 V in 0.5 mol/L Na2SO4 solution. In order to investigate whether the electrode has synergistic effect of electrocatalytic oxidation and membrane filtration, the pyridine simulated wastewater with initial concentration of 100mg/L was treated with the same electrode under the same electrolysis condition in the common plant and the process combination device. The results show that the removal rates of pyridine are 51.96% and 69.89% respectively. The charge efficiency of the latter is high by calculating the instantaneous efficiency of the current. The effects of different initial concentration of pyridine, electrolyte concentration, current density and initial pH value on the removal efficiency of pyridine were investigated to explore the electrocatalytic performance of the prepared electrode. When the electrolyte concentration (anhydrous sodium sulfate) is 10.0 g / L and the current density is 30 mA/cm2,pH=3, the removal rate of 180min from 100mg/L pyridine wastewater is 100%. From the analysis of water samples by UV,HPLC and IC, it is concluded that the process of electrocatalytic oxidation of pyridine by tubular porous Ti/Sb-SnO2 anode also has catalytic oxidation effect on its intermediate products, resulting in the formation of small organic acids, such as formic acid and acetic acid, during the degradation process. The formation of nitrate ion and nitrite ion was also detected. It can be inferred that pyridine breaks the C-N bond on the surface of tubular porous Ti/Sb-SnO2 anode and makes the pyridine ring open and facilitate the subsequent degradation.
【學(xué)位授予單位】：南京理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：O646.54;X703
[Abstract]:Electrocatalytic oxidation (EO) technology has attracted wide attention in the field of environment because of its environmental compatibility and environmental friendliness. The development of high performance anode materials with high electrocatalytic activity and long service life is a hot research topic. The purpose of this paper is to design a reasonable reactor to prepare a porous Ti/Sb-SnO2 tubular membrane electrode with both electrocatalytic activity and membrane filtration performance. In order to improve the electrode performance and charge utilization, it can efficiently catalyze the degradation of pollutants in water. Porous Ti/Sb-SnO2 tubular membrane electrode with different surface microstructure was obtained by using titanium filter tube instead of traditional titanium plate as substrate. The SEM, pore size distribution was characterized by SEM, pore size distribution technique. The grain size of the electrode which could not be prepared by Pechini method and ultrasonic immersion was small. The pore size distribution in porous electrode could be significantly improved by multiple ultrasonic immersion thermal decomposition process, and the average pore size was reduced from 2.607 渭 m to 2.278 渭 m. The results of LSV test showed that the oxygen evolution potential of tubular porous Ti/Sb-SnO2 electrode in acidic, neutral and alkaline media was 2.02V ~ (2.01V), respectively, which could not be prepared by Pechini and ultrasonic immersion, and the results showed that the oxygen evolution potential of tubular porous Ti/Sb-SnO2 electrode was 2.02V ~ (-1) V in acidic, neutral and alkaline media. 1.10V. The pH value of the solution has a great influence on the oxygen evolution potential of the electrode, and the oxygen evolution potential in the alkaline condition is obviously inferior to that in the acidic condition. However, the oxygen evolution potential of the electrode prepared by sol-gel method is only 1.44 V in 0.5 mol/L Na2SO4 solution. In order to investigate whether the electrode has synergistic effect of electrocatalytic oxidation and membrane filtration, the pyridine simulated wastewater with initial concentration of 100mg/L was treated with the same electrode under the same electrolysis condition in the common plant and the process combination device. The results show that the removal rates of pyridine are 51.96% and 69.89% respectively. The charge efficiency of the latter is high by calculating the instantaneous efficiency of the current. The effects of different initial concentration of pyridine, electrolyte concentration, current density and initial pH value on the removal efficiency of pyridine were investigated to explore the electrocatalytic performance of the prepared electrode. When the electrolyte concentration (anhydrous sodium sulfate) is 10.0 g / L and the current density is 30 mA/cm2,pH=3, the removal rate of 180min from 100mg/L pyridine wastewater is 100%. From the analysis of water samples by UV,HPLC and IC, it is concluded that the process of electrocatalytic oxidation of pyridine by tubular porous Ti/Sb-SnO2 anode also has catalytic oxidation effect on its intermediate products, resulting in the formation of small organic acids, such as formic acid and acetic acid, during the degradation process. The formation of nitrate ion and nitrite ion was also detected. It can be inferred that pyridine breaks the C-N bond on the surface of tubular porous Ti/Sb-SnO2 anode and makes the pyridine ring open and facilitate the subsequent degradation.
【學(xué)位授予單位】：南京理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：O646.54;X703
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