本文選題：二乙胺 + N-UNCD��； 參考：《西南科技大學(xué)》2017年碩士論文

【摘要】：摻氮超納米金剛石(N-UNCD)薄膜不僅具備傳統(tǒng)金剛石優(yōu)異的物化性能,而且顯現(xiàn)出納米材料和N型半導(dǎo)體的一些特殊效應(yīng),應(yīng)用前景廣闊。N-UNCD的結(jié)構(gòu)對其宏觀性能影響巨大,深入研究不同結(jié)構(gòu)膜材的制備技術(shù)和性能特點是進(jìn)一步開發(fā)其應(yīng)用的基礎(chǔ)和前提。本文首次采用二乙胺同時作為氮摻雜源和反應(yīng)碳源,通過MPCVD技術(shù)在單晶硅基襯底上制備不同微觀結(jié)構(gòu)的N-UNCD薄膜,利用場發(fā)射掃描電子顯微鏡(SEM)、X射線衍射(XRD)、激光Raman光譜等詳細(xì)表征其微觀形貌、晶體結(jié)構(gòu)和物相組成;在此基礎(chǔ)上采用電化學(xué)分析技術(shù)系統(tǒng)地研究所制備的N-UNCD薄膜的電化學(xué)反應(yīng)活性、雙電層電容及阻抗等性能,并以多巴胺(DA)、抗壞血酸(AA)、金屬銅離子(Cu2+)為研究對象考察N-UNCD薄膜的電化學(xué)檢測能力。結(jié)果表明:(1)以二乙胺為唯一反應(yīng)源可以制備出典型的N-UNCD薄膜,且隨著二乙胺載入量的增加,N-UNCD薄膜的表面形貌從典型的等軸晶粒聚集狀向超納米金剛石晶粒/垂直石墨烯納米墻復(fù)合結(jié)構(gòu)演變,同時薄膜中結(jié)晶石墨相含量明顯增加,導(dǎo)電性顯著增強(qiáng)。(2)N-UNCD薄膜具有優(yōu)于大多數(shù)碳材料的基本電化學(xué)性能,同時不同結(jié)構(gòu)特性的N-UNCD的基本電化學(xué)特性也存在一定的差異。當(dāng)N-UNCD薄膜呈現(xiàn)晶粒聚集狀且石墨相含量較低時,通過[Fe(CN)6]3-/4-為氧化還原探針考察電化學(xué)活性,氧化峰與還原峰峰位差ΔEp值為119mV,隨著薄膜中石墨相含量增加,表面逐漸變?yōu)榻饎偸?垂直石墨墻結(jié)構(gòu)時,ΔEp減小到75 mV,且氧化峰電流強(qiáng)度逐漸增大;而薄膜雙電層電容值則由42.1μF/cm2增加到337.6μF/cm2,同時石墨相含量高的N-UNCD薄膜在10000次充放電測試后,電容值僅下降10.3%;阻抗擬合結(jié)果顯示電荷轉(zhuǎn)移電阻由2486?減小到10.17?,雙電層電容值增大。(3)N-UNCD薄膜對有機(jī)分子和金屬離子具有良好的電化學(xué)檢測能力。較低石墨相含量的薄膜檢測DA,檢測限為8.8μM,隨著薄膜中石墨相增多,檢測限降為0.4μM,還原峰峰電位由+0.35V向+0.175V偏移,線性相關(guān)度均在0.99以上;在檢測AA時,隨膜材結(jié)構(gòu)改變檢測限由12.95μM減小到4.4μM,但線性相關(guān)度也在0.99以上;檢測Cu2+時,石墨相含量較少的薄膜具有更低的檢測限,為0.12ppb,隨著薄膜中石墨相增多,檢測限增大為3.08ppb,線性相關(guān)度0.99降為0.98。(4)N-UNCD薄膜電化學(xué)性能隨膜材結(jié)構(gòu)變化而存在較大的差異,特定組成結(jié)構(gòu)的N-UNCD薄膜電化學(xué)性能優(yōu)異,是一種極具應(yīng)用潛力的電化學(xué)儲能和檢測材料。
[Abstract]:Nitrogen-doped ultrananocrystalline diamond (N-UNCD) thin films not only possess excellent physical and chemical properties of traditional diamond, but also exhibit some special effects of nanomaterials and N-type semiconductors. The structure of N-UNCD has great influence on its macroscopical properties. It is the foundation and prerequisite to further develop the preparation technology and properties of different structure membrane materials. In this paper, diethylamine was used as a nitrogen dopant source and a reactive carbon source for the first time. N-UNCD thin films with different microstructure were prepared on monocrystalline silicon substrates by MPCVD technique. The microstructure, crystal structure and phase composition were characterized by field emission scanning electron microscopy (SEM) and X-ray diffraction (XRD), laser Raman spectroscopy, etc. On the basis of this, the electrochemical reaction activity, double layer capacitance and impedance of N-UNCD thin films prepared by electrochemical analysis were systematically studied. The electrochemical detection ability of N-UNCD thin films was investigated with dopamine (DA), ascorbic acid (AA) and copper ion (Cu2). The results show that the typical N-UNCD films can be prepared by using diethylamine as the sole reaction source. With the increase of loading amount of diethylamine, the surface morphology of N-UNCD film evolves from typical equiaxed grain aggregation to ultrananocrystalline / vertical graphene nanowall composite structure, and the content of crystalline graphite phase in the film increases obviously. The conductivity of N-UNCD thin films is significantly enhanced. The basic electrochemical properties of N-UNCD films are superior to those of most carbon materials. At the same time, the basic electrochemical properties of N-UNCD with different structure are also different. The electrochemical activity of N-UNCD thin films was investigated by [Fe(CN)6] 3 / 4- redox probe when the grain size was aggregated and the graphite phase content was low. The potential difference between the oxidation peak and the reduction peak 螖 E p was 119mV, with the increase of graphite phase content in the film. When the surface becomes diamond / vertical graphite wall structure, 螖 EP decreases to 75 MV, and the current intensity of oxidation peak increases gradually, while the capacitance of double layer increases from 42.1 渭 F/cm2 to 337.6 渭 F / cm 2. At the same time, the N-UNCD film with high graphite phase content increases after 10000 charge-discharge tests. The capacitance value decreased only by 10.3 and the impedance fitting results showed that the charge transfer resistance changed from 2486? When reduced to 10.17 渭 m, the double layer capacitance increases. The thin film has good electrochemical detection ability for organic molecules and metal ions. The detection limit of the thin film with lower graphite phase content is 8.8 渭 m. With the increase of graphite phase in the film, the detection limit decreases to 0.4 渭 M, the peak potential shifts from 0.35V to 0.175V, and the linear correlation is above 0.99. The detection limit decreased from 12.95 渭 M to 4.4 渭 M with the change of membrane structure, but the linear correlation was more than 0.99. In the detection of Cu2, the film with less graphite phase had a lower detection limit of 0.12 ppb, with the increase of graphite phase in the film. The detection limit is increased to 3.08 ppb, and the linear correlation is reduced to 0.99. The electrochemical properties of 0.98.(4)N-UNCD films vary with the structure of the films. The electrochemical properties of N-UNCD films with specific composition are excellent. It is a potential electrochemical energy storage and detection material.
【學(xué)位授予單位】：西南科技大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TQ163;TB383.2

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