本文關(guān)鍵詞：固體氧化物燃料電池中CaO，Pt，，Pd修飾對(duì)氧還原反應(yīng)的增強(qiáng)效應(yīng)　出處：《中國(guó)科學(xué)技術(shù)大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 固體氧化燃料電池 陰極 氧還原反應(yīng) 表面修飾 CaO Pt Pd

【摘要】：能源短缺和環(huán)境污染是全世界在可持續(xù)發(fā)展道路中所面臨的重大問題,因此找到一種高效清潔的能源生產(chǎn)方式迫在眉睫。固體氧化物燃料電池(SOFC)是一種電化學(xué)轉(zhuǎn)換裝置,能高效地將碳?xì)淙剂匣蛘邭淙剂限D(zhuǎn)化成電能,且?guī)缀鯚o污染物的排放。而發(fā)生在陰極的氧還原反應(yīng)(ORR)是影響SOFC性能的主要因素。本論文從提高陰極性能的角度出發(fā),第一部分研究和分析了 CaO修飾對(duì)La0.6Sr0.4Co0.2Fe0.8O3-δ(LSCF)陰極上氧還原反應(yīng)速率的影響;第二部分研究貴金屬Pt和Pd修飾對(duì)La0.7Sr0.3Mn03(LSM)薄膜不同晶面取向上表面交換反應(yīng)過程的影響。以下是本文研究的具體內(nèi)容:第二章中采用離子浸漬法制備CaO修飾的LSCF陰極,探究CaO修飾對(duì)LSCF陰極性能的影響。首先通過向LSCF(LSCF-SDC)電極中浸漬硝酸鈣溶液,800 ℃C熱處理1h后分解得到CaO納米顆粒修飾的LSCF(LSCF-SDC)電極。通過交流阻抗譜分析可知,CaO納米顆粒的修飾可以有效地減小LSCF電極的極化阻抗,且CaO浸漬量為5.18 wt.%時(shí),電極性能最佳。修飾后的CaO-LSCF/SDC/CaO-LSCF對(duì)稱電池在空氣氣氛下650 ℃時(shí)的極化阻抗為0.310Ω·cm2,小于未經(jīng)修飾的0.510 Ω·cm2。并用弛豫時(shí)間分布(DRT)的方法分析交流阻抗譜,發(fā)現(xiàn)通過CaO的浸漬,中頻區(qū)對(duì)應(yīng)的電荷轉(zhuǎn)移過程明顯加快。通過電導(dǎo)弛豫法測(cè)得CaO修飾后LSCF表面交換系數(shù)有一個(gè)數(shù)量級(jí)的增大,當(dāng)0.07 mg·cm-2 的 CaO 涂覆在 LSCF 條子表面時(shí),700℃ 下,Kchem從1.80×10-5cm·s-1增大至2.81×10-4 cm·s-1,表明CaO可促進(jìn)LSCF表面的氧表面交換動(dòng)力學(xué)過程。同時(shí)浸漬電極的單電池上也顯示了良好的性能輸出,濕潤(rùn)H2氣氛下,NiO-SDC/SDC/CaO-LSCF單電池在650℃時(shí)的最大功率密度可達(dá)800 mWcm-2,大于 NiO-SDC/SDC/LSCF 的 600 mWcm-2。第三章中采用不同取向的致密LSM單晶薄膜作為研究對(duì)象,經(jīng)Pt和Pd納米顆粒修飾后,探究貴金屬修飾對(duì)不同取向的LSM薄膜上的氧表面交換反應(yīng)的影響。首先采用脈沖激光沉積(PLD)法制備出(001),(110)和(111)取向的LSM薄膜,然后用蒸鍍法制得Pd和Pt納米顆粒修飾的LSM薄膜上。通過電導(dǎo)弛豫法測(cè)得修飾Pt和Pd修飾前后不同取向的LSM薄膜的表面交換系數(shù),Kchem,測(cè)試溫度區(qū)間為500℃到650℃。發(fā)現(xiàn)未經(jīng)修飾的LSM薄膜,不同晶面取向上的Kchem值不同,且(110)取向在三個(gè)晶面中Kchem值最小,表明三個(gè)晶面上的表面交換動(dòng)力學(xué)過程是不同的。經(jīng)Pd和Pt納米顆粒修飾后,LSM三個(gè)晶面上的Kchem值都增大,表明Pd和Pt對(duì)氧表面交換反應(yīng)動(dòng)力學(xué)都有促進(jìn)作用。且Pd和Pt的促進(jìn)作用不同,其在不同晶面上的提升因子也不相同,且都在(110)取向上最大。Pt修飾的(110)取向的LSM薄膜,其表面交換速率的提升因子高達(dá)129,是Pd修飾的(110)取向的5倍。
[Abstract]:Energy shortage and environmental pollution is a major problem facing the world in the road of sustainable development in an imminent, so to find efficient and clean energy production. The solid oxide fuel cell (SOFC) is an electrochemical conversion device, can efficiently be hydrocarbon fuel or hydrogen fuel into electricity, and almost no pollution and the occurrence of emissions. At the cathode oxygen reduction reaction (ORR) is the main factor affecting the performance of SOFC. This paper focuses on improving the cathode performance point of view, the first part of the research and analysis of CaO modification on La0.6Sr0.4Co0.2Fe0.8O3- 6 (LSCF) on cathodic oxygen reduction reaction rate influence; the second part of the noble metal Pt and Pd modified La0.7Sr0.3Mn03 (LSM) thin films with different crystal orientations on the impact of the surface exchange reaction. The following is the main content of this paper: by ion impregnation method in the second chapter, the preparation of CaO repair LSCF cathode decoration, explore the effects of CaO modification on LSCF cathode performance. Firstly, through to the LSCF (LSCF-SDC) calcium nitrate impregnation solution electrode, LSCF C 800 degrees of heat treatment after 1h decomposition of CaO nanoparticles modified electrode (LSCF-SDC). The AC impedance spectrum analysis shows that the polarization resistance of modified CaO nano particles can be effectively reduce the LSCF electrode, and CaO impregnation was 5.18 wt.%, the best performance. The electrode polarization impedance of CaO-LSCF/SDC/CaO-LSCF symmetric cell modified in the atmosphere at 650 C for 0.310. Cm2, less than the unmodified 0.510. Cm2. and the relaxation time distribution (DRT) method for the analysis of communication impedance spectroscopy, found by CaO impregnation, if the charge transfer process was accelerated. By conductivity relaxation measured by CaO modified LSCF surface exchange coefficient has a magnitude increases, when coated with CaO 0.07 mg - cm-2 Note on LSCF surface, 700 DEG C, from 1.80 Kchem * 10-5cm S-1 * 10-4 cm increased to 2.81 s-1, indicating that CaO can enhance the oxygen surface LSCF surface exchange kinetics. At the same time, single cell immersed electrodes also showed a good performance output, wet H2 atmosphere, NiO-SDC/SDC/ CaO-LSCF in single cell 650 degrees the maximum power density can reach 800 mWcm-2, more than NiO-SDC/SDC/LSCF 600 mWcm-2. in the third chapter, the dense LSM single crystal films with different orientation as the research object, by Pt and Pd nanoparticles modified on noble metal modified effect on oxygen surface exchange reaction of LSM thin films with different orientation. The first by pulsed laser deposition (PLD) was prepared by (001), (110) and (111) oriented LSM films, LSM films and evaporation method of Pd and Pt nanoparticles modified by conductivity relaxation measured by modified Pt and modified Pd not The surface of LSM films with the orientation of the exchange coefficient, Kchem, test the temperature range of 500 C to 650 C. Found that without LSM film modified by different crystal orientations on different Kchem values, and (110) orientation of Kchem in the three planes in the minimum value, show that the surface of the three planes on the exchange the dynamic process is different. The results of Pd and Pt nanoparticles modified LSM three surface Kchem value increased, indicating that Pd and Pt exchange reaction kinetics of oxygen surface have stimulative effect. And the Pd and Pt to promote the role of different, the different crystal on the surface of the lifting factor is not the same. And in the orientation of maximum (110) modified.Pt (110) LSM film orientation, enhance the factor of its surface exchange rate as high as 129, is modified by Pd (110) 5 times the orientation.

【學(xué)位授予單位】：中國(guó)科學(xué)技術(shù)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TM911.4

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