【摘要】：世界范圍內(nèi)對煤、石油、天然氣等化石燃料高效、無污染利用的需求,使得能夠直接使用碳氫燃料發(fā)電的清潔高效發(fā)電裝置——固體氧化物燃料電池(簡稱SOFC)越來越受到人們的重視。多孔電極是固體氧化物燃料電池中非常重要的組成部分,其性能的優(yōu)劣對固體氧化物燃料電池性能的提高起著關(guān)鍵作用。納米復(fù)合電極作為一種新興的多孔電極,由于具有跟電解質(zhì)之間的力學(xué)匹配性高,極化損耗小等優(yōu)點而倍受關(guān)注。盡管納米復(fù)合電極實驗方面的研究很多,理論研究卻相對貧乏,這影響著人們對納米復(fù)合電極內(nèi)部反應(yīng)機理的理解及對其微結(jié)構(gòu)和材料組成的優(yōu)化設(shè)計�？茖W(xué)合理的建立和發(fā)展納米復(fù)合電極的有效性質(zhì)理論,進而建立多物理場模型對納米復(fù)合電極的相關(guān)性能進行對比和優(yōu)化,對實驗研究有非常重要的指導(dǎo)意義。 本論文基于納米復(fù)合電極的實際物理圖像,在傳統(tǒng)電極的有效性質(zhì)理論的基礎(chǔ)上,使用理論推導(dǎo)和多物理場模擬等方法,對具有納米復(fù)合電極結(jié)構(gòu)的固體氧化物燃料電池進行了有效性質(zhì)理論研究和性能模擬優(yōu)化工作,主要內(nèi)容包括如下幾個部分： 在第一章中,我們首先介紹了燃料電池的發(fā)展概況,其次概述了多物理場模擬相關(guān)理論,對建模過程中需要用到的控制方程進行了簡單介紹,進而簡要介紹了納米復(fù)合電極這種新興多孔電極的發(fā)展背景,制作工藝,國內(nèi)外研究現(xiàn)狀以及優(yōu)勢所在,最后我們對理論模擬過程中常見的模擬技術(shù)和方法做了簡要介紹。 第二章從納米復(fù)合電極的幾何結(jié)構(gòu)特殊性出發(fā),引入了多孔電極是由勻質(zhì)導(dǎo)電的等效球隨機排布而成的假設(shè),在已有的由硬球堆積傳統(tǒng)電極電導(dǎo)率理論的基礎(chǔ)上,提出和發(fā)展了納米復(fù)合電極的有效電導(dǎo)率理論,給出了二元納米復(fù)合電極電導(dǎo)率的解析表達式,同時基于三元納米復(fù)合電極中核心骨架的離子傳輸和納米小顆粒之間的離子傳輸形成兩條并聯(lián)的離子傳輸通路的物理圖像,給出了三元納米電極的等效離子電導(dǎo)率表達式,并跟相關(guān)的實驗數(shù)據(jù)進行了比較驗證。 第三章利用有限厚度逾滲閾值的維度理論,對第二章電導(dǎo)率公式中的球殼層電導(dǎo)率進行修正,并用修正后的理論對納米復(fù)合電極的一些特有的實驗現(xiàn)象進行解釋,還進一步討論了層數(shù)因子對球殼層電導(dǎo)率的修正。該電導(dǎo)率理論的計算結(jié)果跟不同Ni的組分,不同溫度和不同電極結(jié)構(gòu)導(dǎo)致的電導(dǎo)率變化的實驗數(shù)據(jù)符合的很好,進一步證明了我們理論的正確性。該理論的提出為納米復(fù)合電極的優(yōu)化設(shè)計奠定了基礎(chǔ)。 第四章發(fā)展了納米復(fù)合電極中的電化學(xué)有效性質(zhì)理論和氣體傳輸有效性質(zhì)理論,分別給出了有效三相線和有效氣孔直徑的解析表達式,并跟實驗數(shù)據(jù)對比,驗證了有效性質(zhì)理論的準(zhǔn)確性,我們還進一步建立了三元納米電極的多物理場模型,對三元納米電極的微結(jié)構(gòu)參數(shù)和電極組分配比做了一系列的討論和優(yōu)化。 第五章基于前面已經(jīng)驗證過的納米復(fù)合電極有效性質(zhì)理論,耦合電子傳輸,離子傳輸,電化學(xué)反應(yīng),氣體傳輸?shù)冗^程建立了不同結(jié)構(gòu)電極對應(yīng)的固體氧化物燃料單電池多物理場模型,該多物理場模型給出的Ⅰ-Ⅴ曲線跟實驗符合的很好,驗證了我們有效性質(zhì)理論的準(zhǔn)確性。對傳統(tǒng)電極,單相浸漬納米電極,雙相浸漬納米電極等不同結(jié)構(gòu)電極的相關(guān)性質(zhì)的比較,使我們對不同結(jié)構(gòu)的多孔電極的優(yōu)缺點有了進一步了解。 第六章對本論文研究內(nèi)容進行簡單的總結(jié)。
[Abstract]:The demand of high efficiency and pollution-free utilization of fossil fuels such as coal, oil and natural gas in the world has made it more and more important to use the clean and high-efficiency power generation device _ solid oxide fuel cell (SOFC) that can directly use hydrocarbon fuel to generate electricity. The porous electrode is a very important component in the solid oxide fuel cell, and the performance of the porous electrode plays a key role in the improvement of the performance of the solid oxide fuel cell. As an emerging porous electrode, the nano-composite electrode is of great concern due to the advantages of high mechanical matching and low polarization loss. In spite of many researches on the experimental aspects of the nano-composite electrode, the theoretical research is relatively poor, which influences the understanding of the internal reaction mechanism of the nano-composite electrode and the optimization design of the microstructure and the material. It is very important to establish and develop the effective property theory of the nano-composite electrode in a scientific and reasonable way, and then to establish the multi-physical field model to compare and optimize the relative performance of the nano-composite electrode. In this paper, based on the actual physical image of the nano-composite electrode, on the basis of the effective property theory of the traditional electrode, the theoretical derivation and the multi-physical field simulation are used. The solid oxide fuel cell with nano-composite electrode structure was studied and the performance of the solid oxide fuel cell was studied. The main contents include the following parts: in chap. I, we first introduce that development of the fuel cell In this paper, the paper briefly introduces the theory of multi-physical field simulation, and briefly introduces the control equation that needs to be used in the modeling process, and then briefly introduces the development background, the manufacturing process, the present situation and the excellent of the new porous electrode of the nano-composite electrode. In the end, we have made a brief introduction to the simulation techniques and methods that are common in the theoretical simulation process In the second chapter, based on the particularity of the geometrical structure of the nano-composite electrode, the assumption that the porous electrode is made from the equivalent ball of homogeneous conduction is introduced. On the basis of the theory of effective conductivity of the nano-composite electrode, the conductivity of the binary nano-composite electrode is given. The expression is analyzed, and meanwhile, the physical image of the two parallel ion transmission paths is formed on the basis of the ion transmission of the core framework in the ternary nano composite electrode and the ion transmission between the nano small particles, and the equivalent ion power of the three-way nano electrode is provided. Expression, and follow the relevant experimental data In the third chapter, the conductivity of the spherical shell in the second conductivity formula is modified by the dimension theory of the percolation threshold of the finite thickness, and some specific examples of the nano-composite electrode are given by the modified theory. The interpretation of the phenomenon is also discussed, and the number of layers of the spherical shell is further discussed. The results of the conductivity theory are in good agreement with the experimental data of the change of conductivity caused by different Ni components, different temperatures and different electrode structures. The theory is based on the optimization of the nano-composite electrode. The paper lays the foundation for the design. The fourth chapter has developed the theory of the electrochemical and effective properties of the nano-composite electrode and the theory of the effective property of the gas transmission. The analytical expression of the effective three-phase line and the diameter of the effective air hole is given, and compared with the experimental data, it is verified that The accuracy of the effect property theory, we have further established the multi-physical field model of the three-way nano-electrode, and the micro-structure parameter and the electrode group distribution ratio of the ternary nano-electrode are compared. A series of discussions and optimization are carried out. The fifth chapter is based on the theory of the effective properties of the nano-composite electrodes that have been verified in the foregoing, and the corresponding solid oxides of different structure electrodes are established in the process of coupling electron transport, ion transport, electrochemical reaction, gas transmission and the like. The multi-physical field model of the fuel cell, the I-V curve given by the multi-physical field model is in good agreement with the experiment, and it is verified that I The accuracy of the theory of effective property is the comparison of the related properties of different structure electrodes, such as the traditional electrode, the single-phase impregnated nano-electrode, the two-phase impregnated nano-electrode, and the like, so that the porous electrode with different structure The advantages and disadvantages of this paper are further understood.
【學(xué)位授予單位】：中國科學(xué)技術(shù)大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2014
【分類號】：TM911.4

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