雙相質(zhì)子—電子混合導(dǎo)體透氫膜的制備及性能研究
發(fā)布時間:2018-02-27 22:06
本文關(guān)鍵詞: 透氫膜 質(zhì)子-電子混合導(dǎo)體 雙相 電導(dǎo)率 化學(xué)穩(wěn)定性 出處:《河北聯(lián)合大學(xué)》2012年碩士論文 論文類型:學(xué)位論文
【摘要】:利用高溫固相法制備出雙相質(zhì)子-電子混合導(dǎo)體BaCe_(0.8)Y_(0.2)O_3/Y_(0.09)Sr_(0.91)TiO_3、BaCe_(0.8)Y_(0.2)O_3/Ce_(0.8)Y_(0.2)O_2、BaCe_(0.8)Y_(0.2)O_3/LaCo_(0.9)Ni_(0.1)O_3。運用X射線衍射、掃描電子顯微鏡和交流阻抗譜法對試樣的相組成、微觀形貌和導(dǎo)電性能進(jìn)行了表征,并對其在4%H_2/Ar、水蒸氣、100%CO_2氣氛中的穩(wěn)定性進(jìn)行了研究。探討了不同氫濃度和溫度對混合導(dǎo)體透氫膜透氫性能的影響,結(jié)果表明: 燒結(jié)溫度及摻雜比例對混合導(dǎo)體相組成和微觀形貌有顯著影響。在一定的燒結(jié)溫度下,三種混合導(dǎo)體均形成了理想的雙相結(jié)構(gòu),沒有雜質(zhì)相的生成;隨著燒結(jié)溫度的提高,晶粒不斷長大,樣品的致密性不斷增大。混合導(dǎo)體BaCe_(0.8)Y_(0.2)O_3/LaCo_(0.9)Ni_(0.1)O_3樣品隨著第二相比例的增加,晶型越來越清晰,單位尺寸的晶界數(shù)量明顯減少。 穩(wěn)定性實驗表明,三種混合導(dǎo)體粉體在含有H_2或水蒸氣的氣氛下是相對穩(wěn)定的,各衍射峰的強度、峰型和峰位置幾乎沒有發(fā)生變化;對CO_2均不夠穩(wěn)定,分解成BaCO_3和CeO_2。 燒結(jié)溫度、摻雜比例、測試氣氛影響混合導(dǎo)體的電性能。在一定的燒結(jié)溫度下,混合導(dǎo)體BaCe_(0.8)Y_(0.2)O_3/Y_(0.09)Sr_(0.91)TiO_3樣品在4%H_2/Ar氣氛下的電導(dǎo)率隨著電子導(dǎo)電相比例的增大而不斷提高,1400℃燒結(jié)的混合導(dǎo)體BaCe_(0.8)Y_(0.2)O_3/Y_(0.09)Sr_(0.91)TiO_3=5/5樣品具有最高的電導(dǎo)率;旌蠈(dǎo)體BaCe_(0.8)Y_(0.2)O_3/Ce_(0.8)Y_(0.2)O_2樣品在不同氣氛下具有不同的導(dǎo)電機制,1550℃燒結(jié)的BaCe_(0.8)Y_(0.2)O_3/Ce_(0.8)Y_(0.2)O_2=3/7樣品在800℃,,4%H_2/Ar氣氛下的電導(dǎo)率最高。1200℃燒結(jié)的不同比例的混合導(dǎo)體BaCe_(0.8)Y_(0.2)O_3/LaCo_(0.9)Ni_(0.1)O_3,在不同的測試氣氛下,表現(xiàn)出不同的導(dǎo)電機制,低溫段,氫氣氣氛下具有最高的電導(dǎo)率,隨著溫度的升高,電子電導(dǎo)成為主要的導(dǎo)電機制,空氣氣氛下的電導(dǎo)率最高。 混合導(dǎo)體BaCe_(0.8)Y_(0.2)O_3/Ce_(0.8)Y_(0.2)O_2透氫結(jié)果顯示,透氫量隨著測試溫度及氫濃度的增加而不斷提高,厚度為1.75mm的3/7樣品,進(jìn)氣為40%H_2/N_2在850℃時的透氫量達(dá)2.4997mL·min~(-1)·cm~(-2)。
[Abstract]:Using the high temperature solid state method, the biphase proton electron mixed conductor BaCeS 0.8YT was prepared. The phase composition of the sample was characterized by X-ray diffraction, scanning electron microscope and AC impedance spectroscopy. The phase composition, microstructure and conductivity of the sample were characterized by means of X-ray diffraction, scanning electron microscope and AC impedance spectroscopy. The phase composition of the sample was characterized by means of X-ray diffraction, scanning electron microscope and AC impedance spectroscopy. The phase composition, microstructure and conductivity of the sample were characterized by X-ray diffraction, scanning electron microscope and AC impedance spectroscopy. The phase composition of the sample was characterized by X-ray diffraction, scanning electron microscope and AC impedance spectroscopy. The phase composition of the sample was characterized by scanning electron microscope and AC impedance spectroscopy. The phase composition of the sample was characterized by means of X-ray diffraction, scanning electron microscope and AC impedance spectroscopy. The phase composition of the sample was characterized by means of X-ray diffraction, scanning electron microscope and AC impedance spectroscopy. The stability of the film in the atmosphere of 4 / H2 / Arh, 100% H _ 2O _ 2 was studied. The effects of different hydrogen concentration and temperature on the hydrogen permeability of the film were discussed. The results show that:. The sintering temperature and doping ratio have a significant effect on the phase composition and micromorphology of the mixed conductors. At a certain sintering temperature, the three kinds of mixed conductors have formed ideal two-phase structure without the formation of impurity phase, and with the increase of sintering temperature, With the increase of the ratio of the second phase, the crystal form of the mixed conductor BaCe_(0.8)Y_(0.2)O_3/LaCo_(0.9)Ni_(0.1)O_3 sample becomes more and more clear, and the number of grain boundaries per unit size decreases obviously. The stability experiments show that the three kinds of mixed conductor powders are relatively stable in the atmosphere containing H _ 2 or water vapor, the intensity, peak type and peak position of each diffraction peak are almost unchanged, and they are not stable to CO_2 and decomposed into BaCO_3 and CeO2. The electric properties of mixed conductors are affected by sintering temperature, doping ratio and test atmosphere. The conductivity of mixed conductor BaCe_(0.8)Y_(0.2)O_3/Y_(0.09)Sr_(0.91)TiO_3 samples sintered at 1400 鈩
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