本文選題：Ti/anoTiO_2薄膜電極　切入點：溶膠凝膠　出處：《安徽理工大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

【摘要】：L-半胱氨酸是一種具有生理功能的含巰基的氨基酸,在生物醫(yī)藥、食品行業(yè)以及生物化妝品領(lǐng)域被廣泛應(yīng)用。用電催化還原L-胱氨酸的方式合成L-半胱氨酸是應(yīng)可持續(xù)發(fā)展的迫切需要而生的一種綠色化工技術(shù)。目前電催化還原L-胱氨酸采用傳統(tǒng)的Pb板,電極催化活性不高且容易造成Pb2+污染,影響產(chǎn)品質(zhì)量,因此尋找一種高催化性能且性能穩(wěn)定的電極是急需解決的問題。Ti02半導(dǎo)體材料在光電催化方面有著非常好的應(yīng)用前景,本文以鈦酸四正丁酯[Ti(OC4H9)4]和稀土的硝酸化合物為原料,采用超聲輔助溶膠-凝膠法制備了稀土La和Ce共摻雜的Ti02薄膜電極(Ti/Ln-nanoTiO2薄膜電極)以及非稀土Sn和稀土La、Ce多摻雜的C薄膜電極(Ti/Ln-nanoSnO2-TiO2薄膜電極)。利用SEM、XRD、XPS以及電化學(xué)測試(CV、EIS)等檢測手段對摻雜改性后的Ti02薄膜電極進行了表征。主要研究成果如下： 1創(chuàng)新了溶膠-凝膠法,首次采用超聲輔助溶膠-凝膠法進行Sn (SnCl4·5H2O)摻雜制備し復(fù)合材料。在實驗中,研究不同超聲時間對Ti/nanoTiO2膜電極的電催化效果的影響,CV測試結(jié)果表明：在超聲15分鐘,頻率為100W時,得到的し薄膜電極的電還原活性最高。同時研究了Sn摻雜量對Ti/nanoSnO2-TiO2膜電極的電催化效果的影響,在優(yōu)化條件下,當Sn摻雜量為1%時,得到的Ti基SnO2-TiO2復(fù)合半導(dǎo)體材料膜電極的電催化還原效果最好,相對于未超聲的電極有更好的催化活性。通過SEM表征發(fā)現(xiàn),其表面顆粒分布相較于未超聲的電極更加均勻。 2在優(yōu)化條件下,以六水合硝酸鑭(La(NO3)3·6H2O)以及六水合硝酸鈰(Ce(NO3)3·6H2O)為稀土摻雜來源,成功實現(xiàn)了Ti02薄膜電極的鑭系共摻雜改性,制備了不同摻雜量的Ti02薄膜電極(Ti/Ln-nanoTiO2薄膜電極)。研究結(jié)果發(fā)現(xiàn)：在lmol/L鹽酸溶液中的CV圖中,當引入的Ce:La:Ti的摩爾比為0.5：0.5：100,所制備的Ti/Ln-nanoTiO2薄膜電極活性是空白電極的6.0倍。 3在優(yōu)化條件下,以六水合硝酸鑭(La(NO3)3-6H2O)、六水合硝酸鈰(Ce(NO3)3·6H2O)為稀土鑭源以及五水合氯化錫(SnCl4·5H2O)為Sn源成功實現(xiàn)了Sn、Ce、La三摻雜改性TiO2,同時制備了不同摻雜組分的Ti02薄膜電極(Ti/nanoSnO2-TiO2、Ti/Ce-nanoSnO2-TiO2、Ti/La-nanoSnO2-TiO2、Ti/Ln-nanoTiO2、 Ti/Ln-nanoSnO2-TiO2薄膜電極)。研究結(jié)果發(fā)現(xiàn)：當引入的Sn:Ce:La:Ti的摩爾比為1：0.5：0.5：100時,所制備的Ti/Ln-nanoSnO2-TiO2薄膜電極活性最高,是空白電極的9.0倍。 4利用Ti/Ln-nanoTiO2薄膜電極,研究了其在L-胱氨酸鹽酸、SnCl2混合溶液中的電催化還原特性及其反應(yīng)機理,結(jié)果表明：Ti/Ln-nanoTiO2薄膜電極在L-胱氨酸SnCl2溶液中的最高峰電流密度為50mA·cm-2,電催化活性是空白Ti/nanoTi02薄膜電極的4.5倍左右。使用Ti/Ln-nanoTiO2薄膜電極進行實驗室電解合成實驗,得到在最佳實驗條件下的電流效率為93.7%,電解產(chǎn)率為91.6%。 5利用Ti/Ln-nanoSnO2-TiO2薄膜電極,研究其在L-胱氨酸溶液中的電催化還原特性及其反應(yīng)機理,結(jié)果表明：Ti/Ln-nanoSnO2-TiO2薄膜電極(Sn:Ce:La:Ti=1：0.5：0.5：100)在L-胱氨酸溶液中的最高峰電流密度為30mA-cm-2,電催化活性是空白Ti/nanoTiO2薄膜電極的4.5倍左右。使用Ti/Ln-nanoSnO2-TiO2薄膜電極進行實驗室電解合成實驗,在最佳實驗條件下,電流效率為85%,L-半胱氨酸鹽酸鹽產(chǎn)率為80%。
[Abstract]:L- is a kind of physiological function of cysteine thiol containing amino acids in biological medicine, food industry and bio cosmetics have been widely applied. The electrocatalytic reduction of L- cystine synthesis L- cysteine is a kind of green chemical technology should be an urgent need for the sustainable development of the students. The electrocatalytic reduction of L- cystine amino acid by traditional Pb board, catalytic activity is not high and it is easy to cause the pollution of Pb2+, affecting the quality of the products, so to find a high catalytic performance and stable performance of the electrode is urgent problem of.Ti02 semiconductor material has a very good prospect in photoelectric catalysis, using butyl titanate four [Ti (OC4H9 4]) and rare earth nitrate compounds as raw materials, Ti02 thin film electrode La and rare earth doped Ce were synthesized by ultrasonic assisted sol-gel method (Ti/Ln-nanoTiO2 films) and non rare earth and Sn Rare earth La, Ce multi doped C thin film electrode (Ti/Ln-nanoSnO2-TiO2 thin film electrode). SEM, XRD, XPS and electrochemical detection (CV, EIS) and other detection methods were used to characterize the modified Ti02 film electrode.
1 innovation of the sol gel method, for the first time by ultrasonic assisted sol-gel method Sn (SnCl4 - 5H2O) were prepared by doping. Composite materials. In the experiment, influence the electrocatalytic effect of different ultrasonic time on Ti/nanoTiO2 membrane electrode, CV test results showed that ultrasound in 15 minutes, at the frequency of 100W. The environmental film electrode electrochemical reduction. The highest activity studied electrocatalytic effect of Sn doping on Ti/nanoSnO2-TiO2 film electrode, under the optimized conditions, when the Sn content was 1%, the electro catalytic Ti based SnO2-TiO2 composite semiconductor film electrode obtained by reduction of the best effect, with respect to the catalytic activity of the electrode without ultrasound the better. The SEM characterization showed that the particle size distribution of surface electrode compared to the non ultrasound is more uniform.
2 under the optimized conditions, with six hydrated lanthanum nitrate (La (NO3) 3 - 6H2O) and six hydrated cerium nitrate (Ce (NO3) 3 - 6H2O) for rare earth doped source, the successful implementation of the Ti02 thin film electrode doped with lanthanide modified Ti02 thin film electrodes were prepared with different doping amount (Ti/ Ln-nanoTiO2 thin film electrode). The results showed that in lmol/L hydrochloric acid solution in the CV diagram, the introduction of Ce:La:Ti when the molar ratio is 0.5:0.5:100, Ti/Ln-nanoTiO2 film electrode preparation is 6 times that of the control electrode.
3 under the optimized conditions, with six hydrated lanthanum nitrate (La (NO3) 3-6H2O), cerium nitrate six hydrate (Ce (NO3) 3 - 6H2O) for rare earth lanthanum source and five tin chloride hydrate (SnCl4 - 5H2O) Sn source for the successful implementation of the Sn, Ce, TiO2 modified La three doped, at the same time preparation of Ti02 thin film electrodes with different doping components (Ti/nanoSnO2-TiO2, Ti/Ce-nanoSnO2-TiO2, Ti/La-nanoSnO2-TiO2, Ti/Ln-nanoTiO2, Ti/Ln-nanoSnO2-TiO2 thin film electrode). The results showed that: when the molar ratio of the Sn:Ce:La:Ti introduced 1:0.5:0.5:100, the prepared Ti/Ln-nanoSnO2-TiO2 thin film electrode was the highest, is 9 times that of the control electrode.
4 using Ti/Ln-nanoTiO2 thin film electrode was investigated in L- cystine hydrochloride, redox properties and reaction mechanism, catalytic SnCl2 mixed solution. The results showed that the peak current density of Ti/Ln-nanoTiO2 thin film electrode in L- cystine SnCl2 solution for 50mA and cm-2, the electrocatalytic activity is about 4.5 times of blank Ti/nanoTi02 thin film electrode the use of Ti/Ln-nanoTiO2 thin film electrode of electrolytic synthesis experiment, current efficiency was obtained under optimal conditions was 93.7%, electrolytic yield is 91.6%.
5 using Ti/Ln-nanoSnO2-TiO2 thin film electrode on the L- cystine solution in the electrocatalytic characteristics and reaction mechanism, the results show that the Ti/Ln-nanoSnO2-TiO2 thin film electrode (Sn:Ce:La:Ti=1:0.5:0.5:100) peak current density in L- cystine in the solution is 30mA-cm-2, the electrocatalytic activity is about 4.5 times of blank Ti/nanoTiO2 thin film electrode using Ti/Ln-nanoSnO2-TiO2 thin films. Electrode for electrolytic synthesis in laboratory experiments, the optimum experimental conditions, the current efficiency was 85% and the yield of 80%. L- cysteine hydrochloride

【學(xué)位授予單位】：安徽理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：O646.54;TB383.1

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