【摘要】：固體氧化物燃料電池(SOFC)由于其能量轉(zhuǎn)換率高、產(chǎn)物無(wú)污染、系統(tǒng)安全性高、模塊化結(jié)構(gòu)等優(yōu)點(diǎn),對(duì)優(yōu)化能源結(jié)構(gòu)、減少環(huán)境污染、促進(jìn)相關(guān)高新技術(shù)產(chǎn)業(yè)的發(fā)展等方面都有著積極的作用,已成為國(guó)際上研究的熱點(diǎn)。氣電共生SOFCs電池可以以烷烴作為燃料氣,質(zhì)子導(dǎo)體型材料作為電解質(zhì),在陽(yáng)極材料的催化作用下,在陰極一側(cè)產(chǎn)生水蒸汽,避免了燃料稀釋的弊端,減小了電池系統(tǒng)的復(fù)雜性,同時(shí)在陽(yáng)極一側(cè)產(chǎn)生具有工業(yè)價(jià)值的化學(xué)中間體烯烴化學(xué)品,這為固體氧化物燃料電池的開(kāi)發(fā)與研究提供新思路。本文在這樣的背景下主要針對(duì)共生SOFCs電解質(zhì)和電極材料的制備及成型工藝進(jìn)行研究。本論文分別采用溶膠凝膠法和高溫固相法制備BaCe_(0.7)Zr_(0.2)Y_(0.1)O_3(BCZY)粉體,探究了溶膠凝膠法和高溫固相法在不同實(shí)驗(yàn)條件下粉體顆粒尺寸的演化情況。通過(guò)對(duì)比實(shí)驗(yàn)得出:當(dāng)乙二胺四乙酸(EDTA)和檸檬酸的添加量與金屬離子摩爾比為1:1.25時(shí),溶膠凝膠法制備的粉體顆粒最小,約25 nm左右;當(dāng)采用高溫固相法制備電解質(zhì)粉體時(shí),以ZrO_2為鋯源,1100℃高溫?zé)Y(jié)6 h的條件下制備的BCZY粉體顆粒較小,約為50 nm,這樣的粉體粒徑有利于后續(xù)電解質(zhì)成型工藝的優(yōu)化。作為共生SOFCs陽(yáng)極材料,氮化釩是一種類(lèi)Pt型催化材料,本研究中對(duì)BCZY粉體熱收縮曲線(xiàn)測(cè)試,對(duì)其燒結(jié)性能進(jìn)行了研究,發(fā)現(xiàn)當(dāng)溫度高達(dá)1590℃時(shí),BCZY粉體均未出現(xiàn)收縮平臺(tái),燒結(jié)性能不夠理想,為此分別采用CuO、ZnO、NiO作為燒結(jié)助劑來(lái)提高電解質(zhì)的燒結(jié)活性,其中CuO效果最佳。論文中探索了不同CuO燒結(jié)助劑添加量對(duì)電解質(zhì)致密性及燒結(jié)溫度的影響,當(dāng)CuO添加量為1.8 wt%,燒結(jié)溫度為1300℃時(shí),電解質(zhì)性能最佳。最后本論文將VN應(yīng)用為共生SOFCs陽(yáng)極材料,通過(guò)實(shí)驗(yàn)研究,采用尿素在氮?dú)鈿夥障聦?duì)偏釩酸銨制備的溶膠凝膠進(jìn)行氮化,在900℃高溫?zé)Y(jié)2 h得到了純相氮化釩(VN)。通過(guò)將CuO與固相法合成BCZY粉體的前驅(qū)體混合、流延、一步燒結(jié)的工藝制備陽(yáng)極支撐電解質(zhì)半電池,采用浸漬法制備陽(yáng)極,絲網(wǎng)印刷法制備陰極得到了陽(yáng)極支撐型全電池,并對(duì)其進(jìn)行了性能測(cè)試,測(cè)試結(jié)果表明電池在700℃時(shí),乙烷轉(zhuǎn)化率為30.8%,乙烯選擇性高達(dá)90.3%,同時(shí),電池的最大功率密度達(dá)到了102 mW cm~(-2)。
[Abstract]:Solid oxide fuel cell (SOFC) has many advantages, such as high energy conversion rate, no pollution, high system safety and modularization structure, so it can optimize energy structure and reduce environmental pollution. Promoting the development of related high-tech industries has played an active role and has become a hot spot in international research. The gas-electric symbiotic SOFCs cell can use alkanes as fuel gas and proton conductor material as electrolyte. Under the catalysis of anode material, water vapor is produced on the cathode side, which avoids the disadvantage of fuel dilution and reduces the complexity of battery system. At the same time, olefin chemicals with industrial value are produced on the anode side, which provides a new idea for the development and research of solid oxide fuel cells. In this context, the preparation and molding process of symbiotic SOFCs electrolytes and electrode materials were studied. In this paper, BaCe_ (0.7) Zr_ (0.2) Y _ (0.1) O _ 3 (BCZY) powders were prepared by sol-gel method and high-temperature solid-state method, respectively. The particle size evolution of sol-gel method and high-temperature solid-state method under different experimental conditions was investigated. The results show that when the molar ratio of ethylenediamine tetraacetic acid (EDTA) and citric acid to metal ion is 1: 1.25, the particle size prepared by sol-gel method is about 25 nm. When the electrolyte powder was prepared by high temperature solid state method, ZrO_2 was used as zirconium source and the size of BCZY powder sintered at 1100 鈩，

本文編號(hào)：2317370