本文選題：銅銠基氧化物 + 熱電材料�。� 參考：《昆明理工大學(xué)》2017年碩士論文

【摘要】：隨著社會(huì)的高速發(fā)展,人類(lèi)對(duì)能源需求量日益增加。尤其是進(jìn)入21世紀(jì)以來(lái),城市化和工業(yè)化的日益普及,能源危機(jī)更加嚴(yán)峻,環(huán)境污染愈顯突出,已成為當(dāng)今世界的兩大難題。因此,尋找新型能源和新型能源材料,勢(shì)在必行。熱電材料是一種能實(shí)現(xiàn)熱能和電能直接相互轉(zhuǎn)化的新型環(huán)保型功能材料。熱電材料尤其是氧化物熱電材料具有無(wú)毒、無(wú)污染、無(wú)噪音、高溫穩(wěn)定性好等優(yōu)點(diǎn),在廢熱回收利用、太陽(yáng)能吸收、以及熱管理等方面具有廣泛的應(yīng)用前景。因此,近年來(lái),熱電材料已引起了廣大研究者的密切關(guān)注。本文首先對(duì)熱電材料的研究進(jìn)展及應(yīng)用前景等問(wèn)題進(jìn)行了闡述。然后以銅銠基氧化物熱電材料為研究對(duì)象,計(jì)算了摻雜元素對(duì)其晶格熱導(dǎo)率的影響,討論了熱電材料的制備方法、物理特性、性能表征、以及影響熱電性能的參數(shù)。并通過(guò)摻雜改性對(duì)銅銠基熱電氧化物熱電材料的性能進(jìn)行了系統(tǒng)研究。主要研究?jī)?nèi)容和實(shí)驗(yàn)結(jié)果可概括如下:簡(jiǎn)單介紹了實(shí)驗(yàn)中需要用到的熱電性能參數(shù)主要測(cè)試儀器(鎢燈絲掃描電子顯微鏡、X射線衍射儀、激光熱導(dǎo)儀、高性能全自動(dòng)賽貝克系數(shù)-電導(dǎo)測(cè)試系統(tǒng))及其測(cè)試原理。利用 CASTEP 程序?qū)?CuRh2-2xM2xO4 和 CuRh1-yMyO2(M=Cr、Co、Mg,x、y=0,0.05,0.1,0.15,0.2,0.25,0.3)的晶格熱導(dǎo)率進(jìn)行了第一性原理計(jì)算,得出以下結(jié)論:三種摻雜元素均可降低材料的晶格熱導(dǎo)率,材料的晶格熱導(dǎo)率也隨著摻雜量的上升而下降,而且Mg元素?fù)诫s對(duì)降低晶格熱導(dǎo)率的效果最好。研究了樣品制備工藝,結(jié)果表明:CuRh02是CuRh204的高溫相,940℃C和980℃分別為CuRh2-2xMg2xO4和CuRh1-yMgyO2的最佳燒結(jié)溫度,并通過(guò)固相反應(yīng)法成功制備出了摻雜樣品;但為了提高熱電性能與檢測(cè)需要,繼續(xù)對(duì)各樣品進(jìn)行了放電等離子燒結(jié)。采用二步固相反應(yīng)-放電等離子燒結(jié)法通過(guò)Rh位摻雜Mg位摻雜得到了一系列CuRh2-2xMg2xO4塊體樣品。分析了摻雜對(duì)材料的物相、形貌以及熱電性能的影響。實(shí)驗(yàn)結(jié)果表明:微量摻雜對(duì)基體的結(jié)構(gòu)和物相影響較小,當(dāng)x0.25時(shí),晶界間可能有第二相析出,影響了材料的電學(xué)性能,導(dǎo)致功率因子下降。CuRh2.2xMg2xO4的熱導(dǎo)率、賽貝克系數(shù)、電導(dǎo)率均隨摻雜量的上升而下降,功率因子最高的是CuRh1.6Mg0.404(在 900℃下達(dá)到了 165.53 μ W/mK-2),但 ZT 值最高的是 CuRh1.5Mg0.5O4,在 900℃時(shí)ZT最大值為:0.18。采用二步固相反應(yīng)-放電等離子燒結(jié)法制備了 一系列CuRh1-yMgyO2塊體樣品,并對(duì)其熱電性能進(jìn)行了表征測(cè)試。實(shí)驗(yàn)結(jié)果表明:制備粉末具有明顯的層狀結(jié)構(gòu)。經(jīng)過(guò)SPS燒結(jié)處理后,塊體樣品的致密度達(dá)理論密度的90%以上,晶粒尺寸隨著Mg摻雜量的增加而減小。樣品的熱導(dǎo)率均隨摻雜量的上升而下降,但賽貝克系數(shù)和電導(dǎo)率均隨摻雜量的上升而上升。CuRh0.7Mg0.3O2的ZT值最高,900℃時(shí)最大值為0.21。本論文較為系統(tǒng)的研究了銅銠基氧化物熱電材料,利用制備工藝、Mg元素?fù)诫s等手段,不同程度的提高了其熱電性能。研究結(jié)果表明銅銠基氧化物熱電材料是一種很有潛質(zhì)的材料體系,具有較高的研究?jī)r(jià)值和應(yīng)用前景;同時(shí)為研發(fā)高性能氧化物熱電材料提出了可供借鑒的理論支持和技術(shù)參考。
[Abstract]:With the rapid development of society, human demand for energy is increasing. Especially since twenty-first Century, the increasing popularity of urbanization and industrialization, the energy crisis is more severe, the environmental pollution is becoming more and more prominent, and it has become the two major problem in the world. Therefore, it is imperative to find new energy sources and new energy materials. The thermoelectric materials, especially oxide thermoelectric materials, have the advantages of non-toxic, pollution-free, no noise, high temperature stability, etc., and have extensive application prospects in waste heat recovery, solar absorption, and heat management. The research progress and application prospect of thermoelectric materials have been discussed in this paper. Then, the effects of the doped elements on the thermal conductivity of the lattice are calculated, and the preparation methods, physical properties and performance characterization of the thermoelectric materials are discussed. The properties of copper rhodium based thermoelectric thermoelectric materials are systematically studied by doping modification. The main research contents and experimental results can be summarized as follows: the main testing instruments used in the experiment are briefly introduced (tungsten filament scanning electron microscope, X ray diffractometer, excitation). Photothermal conductance, high performance fully automatic Seebeck coefficient - conductance test system and its testing principle. Using the CASTEP program, the thermal conductivity of CuRh2-2xM2xO4 and CuRh1-yMyO2 (M=Cr, Co, Mg, x, y=0,0.05,0.1,0.15,0.2,0.25,0.3) is calculated by the first principle, and the conclusion is that three kinds of doping elements can reduce the lattice heat of the material. The thermal conductivity of the material decreases with the increase of the doping amount, and the effect of doping Mg elements to reduce the thermal conductivity of the lattice is the best. The preparation process of the sample is studied. The results show that CuRh02 is the high temperature phase of CuRh204 and the optimum sintering temperature of CuRh2-2xMg2xO4 and CuRh1-yMgyO2 at 940, C and 980, respectively, and by the solid state reaction method. The doped samples were successfully prepared, but in order to improve the thermoelectric properties and detection needs, the samples were continuously sintered by discharge plasma. A series of CuRh2-2xMg2xO4 bulk samples were obtained by doping the Rh bit doping Mg bit with the two step solid state reaction discharge plasma sintering method. The phase, morphology and thermoelectric properties of the doped materials were analyzed. The experimental results show that micro doping has little influence on the structure and phase of the matrix. When x0.25, there may be a second phase precipitation between the grain boundaries, which affects the electrical properties of the material, which leads to the decrease of the thermal conductivity of the power factor of the.CuRh2.2xMg2xO4, the asbeck coefficient and the electrical conductivity are all decreased with the increase of the doping amount, and the highest power factor is the increase of the power factor. CuRh1.6Mg0.404 (reached 165.53 W/mK-2 at 900 C), but the highest ZT value is CuRh1.5Mg0.5O4. At 900, the maximum ZT value is: 0.18. using two step solid state reaction discharge plasma sintering method to prepare a series of CuRh1-yMgyO2 block samples, and the thermoelectric properties are characterized and tested. The experimental results show that the powder is prepared. After SPS sintering, the density of the sample is more than 90% of the theoretical density, and the grain size decreases with the increase of Mg doping. The thermal conductivity of the sample decreases with the increase of the doping amount, but the Sibeck coefficient and the conductivity increase with the doping amount and the ZT value of.CuRh0.7Mg0.3O2 is the highest, 900. The maximum value of C (0.21.) is a systematic study of copper rhodium oxide thermoelectric materials. The thermoelectric properties are improved by means of preparation technology and Mg element doping. The results show that the copper rhodium oxide thermoelectric material is a very latent material system, which has high research value and application prospect. At the same time, it provides a theoretical support and technical reference for developing high performance oxide thermoelectric materials.

【學(xué)位授予單位】：昆明理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類(lèi)號(hào)】：TB34

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