發(fā)布時(shí)間：2018-11-05 13:36

【摘要】：硫-氧固體氧化物燃料電池(SOFC)是一種以硫磺蒸汽或者SO2替代氫氣作為燃料的新型全固態(tài)能量轉(zhuǎn)換裝置。目前,SOFC電池堆的結(jié)構(gòu)主要分為平板式以及管式兩種。相比較而言,平板式SOFC具有電性能良好、制造簡(jiǎn)單、成本低等優(yōu)點(diǎn),是當(dāng)前SOFC研究的熱點(diǎn)。而作為SOFC的重要組成部分,如何利用簡(jiǎn)單、低廉的方法制備出高性能的電解質(zhì)薄片引起了越來(lái)越多研究者的關(guān)注。本文主要研究了不同制備條件對(duì)硫-氧SOFC電解質(zhì)片的性能影響,并對(duì)硫-氧SOFC單電池的制備以及電池堆的設(shè)計(jì)制造進(jìn)行了初步的探索研究。(1)通過(guò)溶膠-凝膠法分別制備了La0.8Pr0.2CrO3以及La0.7Sr0.3MnO3(LSM)粉體作為硫-氧SOFC的陽(yáng)極及陰極催化劑,并對(duì)所制備的粉體進(jìn)行了XRD以及SEM表征。(2)使用聚醚砜作為硫-氧SOFC電解質(zhì)成型溶劑,利用正交實(shí)驗(yàn)方法安排制備出不同實(shí)驗(yàn)條件下的電解質(zhì)薄片,采用涂覆的方法在薄片兩側(cè)均勻涂覆陰極、陽(yáng)極漿料,經(jīng)干燥燒結(jié)形成“陰極/絲網(wǎng)‖電解質(zhì)‖絲網(wǎng)/陽(yáng)極”單片電池結(jié)構(gòu),組裝出單電池發(fā)電系統(tǒng)。以硫蒸汽作為燃料氣體,對(duì)不同電解質(zhì)片所構(gòu)成的單電池進(jìn)行電性能測(cè)試,通過(guò)結(jié)果分析得到硫-氧SOFC電解質(zhì)片的最佳制備工藝:電解質(zhì)粉體與聚醚砜的配比選擇5:1(g/mL)、Na2SO4混合電解質(zhì)粉體的質(zhì)量百分比選擇25wt%、電解質(zhì)粉體的類(lèi)型選擇5 mol%氧化釔穩(wěn)定的氧化鋯(5YSZ)、復(fù)合電解質(zhì)片的預(yù)燒溫度選擇400℃。將采用最佳制備工藝得到的電解質(zhì)片組裝成單電池,對(duì)其進(jìn)行電性能測(cè)試,該單電池在780℃獲得最大開(kāi)路電壓814 mV,當(dāng)電池的電流密度達(dá)到93 mA/cm2時(shí),獲得最大功率密度37.7mW/cm2。(3)選用304不銹鋼作為電池框架,將復(fù)合單片電池依次插入框架的間隔槽內(nèi),經(jīng)密封后構(gòu)成Ⅰ-型電池堆,以硫磺蒸汽作為燃料氣體,對(duì)Ⅰ-型電池堆進(jìn)行測(cè)試,結(jié)果表明,該電池堆在760℃獲得最大開(kāi)路電壓697 mV;經(jīng)20 h不間斷工作后,電池的開(kāi)路電壓衰減率為5.6%;經(jīng)10次熱沖擊循環(huán)后,電池堆開(kāi)路電壓衰減率達(dá)到50.7%;當(dāng)電池堆的輸出電流密度為104 mA/cm2時(shí),電池堆的獲得最大功率密度33.3 mW/cm2。(4)采用“不銹鋼框架-電解質(zhì)”一體化結(jié)構(gòu),配合電池墊片,經(jīng)螺栓壓實(shí)、密封膠密封最終得到Ⅱ-型電池堆,以硫磺蒸汽作為燃料氣體,對(duì)Ⅱ-型電池堆進(jìn)行測(cè)試,結(jié)果表明,電池堆在770℃達(dá)到最大開(kāi)路電壓753 mV;經(jīng)20 h不間斷工作,電池堆的開(kāi)路電壓衰減率為10.4%;經(jīng)10次熱沖擊循環(huán)后,電池堆開(kāi)路電壓衰減率僅為9.4%;當(dāng)輸出電流密度為109 mA/cm2時(shí),Ⅱ-型電池堆的獲得最大功率密度39.4 mW/cm2,略高于Ⅰ-型電池堆,相比較而言,Ⅱ-型電池堆的性能得到了較大程度的改善。
[Abstract]:Sulfur-oxygen solid oxide fuel cell (SOFC) is a new all solid state energy conversion device which uses sulfur vapor or SO2 instead of hydrogen as fuel. At present, the structure of SOFC battery stack is mainly divided into flat type and tube type. In contrast, flat SOFC has the advantages of good electrical performance, simple manufacturing and low cost, so it is a hot spot in current SOFC research. As an important part of SOFC, how to prepare high performance electrolyte sheet by simple and low cost method has attracted more and more researchers' attention. In this paper, the effects of different preparation conditions on the properties of SOFC electrolytes were studied. The preparation of sulfur-oxygen SOFC single cell and the design and manufacture of the battery stack were studied. (1) La0.8Pr0.2CrO3 and La0.7Sr0.3MnO3 (LSM) powder were prepared by sol-gel method respectively as the sulfur- Anode and cathode catalysts for oxygen SOFC, The prepared powders were characterized by XRD and SEM. (2) Polyether sulfone was used as the solvent for the formation of SOFC electrolytes, and the electrolyte sheets were prepared under different experimental conditions by orthogonal experimental method. The cathode and anode paste were evenly coated on both sides of the thin sheet by coating method. The single cell structure was formed by drying and sintering, and the single cell generation system was assembled. Using sulfur vapor as fuel gas, the electric performance of a single cell composed of different electrolytes was tested. Through the analysis of the results, the optimum preparation process of SOFC electrolyte sheet was obtained: the ratio of electrolyte powder to polyether sulfone was 5:1 (g/mL), the mass percentage of mixed electrolyte powder of Na2SO4 was 25 wts. The type of electrolyte powder is 5 mol% yttrium stabilized zirconia (5YSZ), and the pre-firing temperature of composite electrolyte is 400 鈩，

本文編號(hào)：2312250