本文選題：摩擦納米發(fā)電機 + 自驅(qū)動　； 參考：《河南師范大學》2017年碩士論文

【摘要】：有機污染物對生物體和環(huán)境具有極大的危害性,預防、控制和治理有機物污染已成為當前備受關注的問題。電化學法作為一種理想的處理廢水有機污染物的方法,可以在短時間內(nèi)將毒性大、難降解的有機污染物處理成無毒或無二次污染的完全降解物。然而,傳統(tǒng)的電化學降解裝置靠外部能源驅(qū)動,外部能源主要來自煤、石油等化石燃料,這無疑在加重能源負擔的同時,造成了新的環(huán)境污染,也極大限制了電化學降解在污染物處理中的廣泛應用。摩擦納米發(fā)電機(Triboelectric Nanogenerator,TENG)是一種基于摩擦帶電和靜電感應原理的新型能源轉(zhuǎn)化裝置,能將環(huán)境中種類繁多的閑散、無用、甚至影響人類生活的機械能轉(zhuǎn)換成電能,相對于傳統(tǒng)的發(fā)電機,具有質(zhì)量輕、體積小、選材廣、造價低等優(yōu)點。將TENG和電化學有機污染物處理裝置相結(jié)合,組成自驅(qū)動電化學降解系統(tǒng),借助水流、風能、人體運動等自然界中紛繁復雜的機械振動驅(qū)動TENG工作,不僅能夠?qū)崿F(xiàn)環(huán)境中機械能的收集利用,而且能夠在一定程度上解決低濃度有機物污染的問題。因此,基于TENG的自驅(qū)動電化學裝置在廢水有機物處理中具有廣闊的應用前景。本論文基于摩擦納米發(fā)電機的自驅(qū)動電化學系統(tǒng)在有機污染物處理中的應用展開研究。主要完成以下三個目標:(1).設計構建輸出效率高、廉價、易于調(diào)控的TENG;(2).基于設計的TENG開展自驅(qū)動電化學系統(tǒng)在有機污染物處理中的應用;(3).深入研究相關有機污染物的消除過程和消除機理�；谏鲜瞿繕�,我們完成了如下研究工作:(1)設計出交叉折疊結(jié)構的新型摩擦納米發(fā)電機(PICL-TENG),并首次將自驅(qū)動電化學系統(tǒng)應用于苯胺類有機物的氧化聚合。通過螺絲和彈簧將多個摩擦單元鉸接,成功制作出基于平面滑動模式的新型交叉折疊結(jié)構的TENG。隨后,借助高壓電荷注入技術增加摩擦層表面電荷密度,有效提升了PICL-TENG的輸出性能,使其開路電壓、短路電流和峰功率密度分別達到845.6 V、69.9μA和1.59 W m-2。選取苯胺、N-羥乙基苯胺、三(4-溴苯)胺這三種具有不同取代基的苯胺類有機物作為研究對象,依靠PICL-TENG供能,成功使苯胺類有機物發(fā)生電化學氧化。同時,研究結(jié)果表明,PICL-TENG作為供能系統(tǒng),在任何季節(jié)均能實現(xiàn)苯胺類有機物的氧化,進而拓展了自驅(qū)動電化學體系的應用范圍。(2)構建出多層聯(lián)動結(jié)構的新型摩擦納米發(fā)電機(PMLL-TENG),并成功應用于自驅(qū)動甲基黃染料的電化學氧化降解。借助連桿和螺絲將多個摩擦單元并聯(lián),制作成多個摩擦層可以同時接觸和分離的多層聯(lián)動結(jié)構的TENG。通過對PTFE膜進行電荷注入處理,其平均開路電壓、短路電流和峰功率密度分別提升至793 V、0.56 mA和30.8 W m-2。在PMLL-TENG驅(qū)動的電化學體系中,高毒性的甲基黃染料最終完全降解為二氧化碳。此外,以循環(huán)伏安、氣相色譜-質(zhì)譜聯(lián)用和核磁共振氫譜等技術為研究手段,對其氧化過程和機理進行探究,初步探索出甲基黃的降解是通過陽極界面處產(chǎn)生的活性氧如HO·,攻擊與-N=N-相鄰的C-N鍵,最終間接氧化降解為CO2。(3)制作出旋轉(zhuǎn)圓盤結(jié)構的摩擦納米發(fā)電機(rd-TENG),并成功用于4-氨基偶氮苯的自驅(qū)動電化學氧化降解或聚合。首次使用鋁塑板做電極和基底,通過對鋁塑板和亞克力板進行雕刻處理,制作出具有精美圖案的定子和轉(zhuǎn)子,進而組裝成旋轉(zhuǎn)圓盤結(jié)構的TENG。用電動裝置模擬自然界中的機械能,研究出轉(zhuǎn)速和rd-TENG輸出性能的關系。利用rd-TENG輸出的電能,4-氨基偶氮苯可以選擇性氧化為聚合物或二氧化碳。通過分析不同電壓區(qū)間和掃速的循環(huán)伏安圖像,結(jié)合交流阻抗、氣相色譜-質(zhì)譜聯(lián)用、紫外吸收光譜等技術,分析4-氨基偶氮苯的降解/聚合過程:在低電壓下,4-氨基偶氮苯聚合成低聚物;在高電壓下,通過陽極界面產(chǎn)生的活性物如HOCl/Cl2快速攻擊-N=N-鄰位的C-N,并在-NH2的鄰位親核取代苯環(huán)上的氫,HOCl/Cl2進一步氧化生成的中間物直至降解為CO2。據(jù)此,可以通過合理控制電化學氧化電位對AAB進行降解或聚合,這對有機污染物的處理具有指導意義。
[Abstract]:Organic pollutants have great harm to organisms and the environment. Prevention, control and control of organic pollutants have become an issue of great concern. As an ideal method of treating organic pollutants in wastewater, electrochemical method can treat organic pollutants with large toxic and difficult degradation into non-toxic or no two pollution in a short time. However, the traditional electrochemical degradation device is driven by external energy, and the external energy is mainly from coal, petroleum and other fossil fuels, which undoubtedly aggravates the energy burden, resulting in new environmental pollution, and it also greatly restricts the extensive application of electrochemical degradation in the treatment of pollutants. Triboelectr IC Nanogenerator, TENG) is a new type of energy conversion device based on the principle of friction electrification and electrostatic induction. It can convert a wide variety of idle, useless, and even influence the mechanical energy of human life into electrical energy. Compared with the traditional generator, it has the advantages of light quality, small size, wide selection of materials and low cost. The machine pollutant treatment device combines the self driving electrochemical degradation system to drive TENG with the help of the complicated mechanical vibration in nature, such as water flow, wind energy, human body movement and so on. It can not only realize the collection and utilization of mechanical energy in the environment, but also solve the problem of low concentration organic matter to a certain extent. Therefore, based on TE NG's self driven electrochemical device has a broad application prospect in the treatment of wastewater organic matter. This paper is based on the application of the self driven electrochemical system of friction nanoscale in the treatment of organic pollutants. The following three objectives are completed: (1). The design and construction of high efficiency, cheap, easy to regulate and control of TENG; (2). TENG is used to carry out the application of self driven electrochemical system in the treatment of organic pollutants; (3) in-depth study of the elimination process and elimination mechanism of related organic pollutants. Based on the above objectives, we have completed the following research work: (1) a new type of friction nanoscale generator (PICL-TENG) is designed for the first time, and the self driven electrification is the first time. The system is applied to the oxidation polymerization of aniline organic matter. A number of friction units are hinged by screws and springs. A new type of cross folded structure TENG. based on plane sliding mode is successfully produced. The charge density of the surface of the friction layer is increased by the high pressure charge injection technology, which can improve the output performance of PICL-TENG and make it open. Voltage, short circuit current and peak power density reach 845.6 V, 69.9 mu A and 1.59 W m-2. to select aniline, N- hydroxyethyl aniline, three (4- bromine) amine, which have different substituents of aniline as the research object, and rely on PICL-TENG to supply energy, the aniline type machine can be electrochemical oxidation. At the same time, the results show PICL-TE NG, as an energy supply system, can realize the oxidation of aniline like organic matter in any season, and then expand the application scope of the self driven electrochemical system. (2) a new type of friction nanoscale generator (PMLL-TENG) is constructed and applied to the electrochemical oxidation degradation of self driving methyl yellow dye. The friction unit is connected in parallel, and TENG. is injected into the PTFE film by the multi-layer linkage with multiple friction layers. The average open circuit voltage, short circuit current and peak power density are increased to 793 V, 0.56 mA and 30.8 W m-2. in PMLL-TENG driven electrochemical system, with high toxic methyl yellow. The dye finally completely degraded to carbon dioxide. In addition, the oxidation process and mechanism were explored by cyclic voltammetry, gas chromatography mass spectrometry combined with nuclear magnetic resonance spectroscopy. The degradation of methyl yellow was preliminarily explored as the active oxygen, such as HO, produced by the anode interface, attacking the C-N bonds adjacent to -N=N-, and ultimately indirectly. The friction nanoscale generator (rd-TENG) was produced by the oxidation degradation of CO2. (3), and it was successfully used for the self driven electrochemical oxidation degradation or polymerization of 4- amino azobenzene. The aluminum plastic plate was first used as the electrode and substrate. The stators and rotors with fine patterns were made by engraving the aluminum plastic plate and acrylic plate. The TENG., which is assembled into a rotating disk structure, simulates the mechanical energy in nature with an electric device, and studies the relationship between the rotational speed and the output performance of the rd-TENG. The 4- amino azobenzene can be selectively oxidized to polymer or carbon dioxide by using the output of rd-TENG. Impedance, gas chromatography-mass spectrometry (GC-MS), UV absorption spectroscopy and other techniques to analyze the degradation / polymerization process of 4- amino azobenzene: at low voltage, 4- amino azobenzene is polymerized into oligomers; at high voltage, the active substances produced by the anode interface, such as HOCl/Cl2, quickly attack the C-N of the -N=N- neighborhood, and replace the hydrogen on the benzene ring in the neighborhood of the -NH2. HOCl/Cl2 can be further oxidized and degraded into CO2., and the AAB can be degraded or polymerized by reasonable control of electrochemical oxidation potential, which is of guiding significance for the treatment of organic pollutants.

【學位授予單位】：河南師范大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X703;O646

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