【摘要】：太陽(yáng)能利用以其儲(chǔ)量無(wú)限性、開(kāi)發(fā)利用清潔性,成為21世紀(jì)解決化石能源短缺、環(huán)境污染和溫室效應(yīng)等問(wèn)題的有效途徑之一。太陽(yáng)能高溫?zé)峄瘜W(xué)轉(zhuǎn)換是通過(guò)聚光產(chǎn)生高溫?zé)崮軄?lái)驅(qū)動(dòng)熱化學(xué)反應(yīng),將所聚集的太陽(yáng)能轉(zhuǎn)化為碳?xì)淙剂系幕瘜W(xué)能,并在制氫、溫室氣體減排等領(lǐng)域得到廣泛的研究與應(yīng)用。太陽(yáng)能與熱化學(xué)反應(yīng)相結(jié)合的能量轉(zhuǎn)換過(guò)程不僅使其由物理能品位提升到化學(xué)能品位,而且可以將太陽(yáng)能存儲(chǔ)為解決單獨(dú)光熱利用系統(tǒng)不穩(wěn)定、不連續(xù)等問(wèn)題,有效提高太陽(yáng)能熱利用系統(tǒng)的效率。相比于其他制氫工質(zhì)對(duì),鐵酸鹽(MFe_2O_4,M=Ni,Co,Cu,Zn等)工質(zhì)對(duì)由于其熱解溫度較低、氧化還原性能良好以及具有較高的產(chǎn)氫率而受到了人們的青睞。本文以兩步熱化學(xué)循環(huán)制氫為應(yīng)用背景,結(jié)合實(shí)際應(yīng)用過(guò)程中對(duì)太陽(yáng)能高效低成本利用技術(shù)的發(fā)展需求,分析了太陽(yáng)能熱化學(xué)轉(zhuǎn)換技術(shù)中光-熱-化學(xué)能輸運(yùn)特性,采用數(shù)值模擬與實(shí)驗(yàn)測(cè)量相結(jié)合的手段研究了聚集太陽(yáng)輻射熱解鐵酸鹽顆粒過(guò)程中光熱傳輸特性。主要的研究?jī)?nèi)容如下:采用化學(xué)共沉淀法制備了適用于中高溫太陽(yáng)能熱化學(xué)制氫的鐵酸鹽微顆粒(Ni Fe_2O_4、Cu Fe_2O_4、Mn_(0.9)Cu_(0.1)Fe_2O_4),采用XRD、SEM等手段獲得了制備顆粒的純度、粒徑、孔隙度等參數(shù);通過(guò)同步熱分析儀獲得了不同加熱速率下Ni Fe_2O_4和Cu Fe_2O_4顆粒的失重曲線以及初始分解溫度;基于失重曲線采用Flynn-Wall-Ozawa方法得到了Ni Fe_2O_4和Cu Fe_2O_4顆粒的熱分解動(dòng)力學(xué)三參數(shù):表觀活化能、指前因子和機(jī)理函數(shù)。搭建了用于能源材料光譜輻射物性測(cè)量的實(shí)驗(yàn)裝置,通過(guò)中國(guó)計(jì)量院的標(biāo)準(zhǔn)樣片實(shí)驗(yàn)數(shù)據(jù)獲得了實(shí)驗(yàn)系統(tǒng)的測(cè)量誤差以及測(cè)量不確定度。采用溴化鉀壓片法測(cè)量了鐵酸鹽微顆粒在光譜區(qū)間0.5-2.1μm的光譜透過(guò)特性;運(yùn)用Mie理論和KK關(guān)系式反演獲得了鐵酸鹽粒子的復(fù)折射率與光譜的變化關(guān)系;基于計(jì)算得到復(fù)折射率,采用普朗克平均因子法分析了鐵酸鹽顆粒平均吸收因子與溫度的變化關(guān)系。建立了多層-多碟聚光器的光輸運(yùn)模型,校正了多碟系統(tǒng)設(shè)計(jì)參數(shù)并分析了太陽(yáng)能多碟聚光系統(tǒng)焦平面熱流的分布規(guī)律,揭示了太陽(yáng)能多碟聚光系統(tǒng)中反射鏡固定螺栓遷移對(duì)聚集熱流散斑的影響機(jī)理。采用蒙特卡洛法與有限體積法建立太陽(yáng)能熱裂解金屬氧化物顆粒過(guò)程中熱化學(xué)反應(yīng)流的光熱輸運(yùn)模型,分析了Ni Fe_2O_4反應(yīng)顆粒粒徑、質(zhì)量流量、保護(hù)氣體流速以及溫度等對(duì)反應(yīng)器內(nèi)溫度場(chǎng)、流場(chǎng)分布以及反應(yīng)顆粒轉(zhuǎn)化率的影響;研制了腔式太陽(yáng)能熱化學(xué)反應(yīng)器,分析了運(yùn)行參數(shù)對(duì)反應(yīng)腔熱性能的影響,獲得了太陽(yáng)直射熱流密度以及保護(hù)氣體流量對(duì)反應(yīng)器內(nèi)壁面溫度的影響規(guī)律。采用?理論并結(jié)合UDF技術(shù)數(shù)值分析了太陽(yáng)能熱化學(xué)反應(yīng)器在不同工況參數(shù)(反應(yīng)顆粒粒徑、質(zhì)量流量、保護(hù)氣體流速以及溫度等)時(shí)物理?和化學(xué)?的分布特性;考慮理想Ni Fe_2O_4和Cu Fe_2O_4工質(zhì)對(duì)太陽(yáng)能熱化學(xué)系統(tǒng),采用熱力學(xué)第二定律研究了不同工況參數(shù)對(duì)系統(tǒng)效率以及太陽(yáng)能-化學(xué)能轉(zhuǎn)化效率的影響;研究結(jié)果為太陽(yáng)能熱化學(xué)反應(yīng)器的優(yōu)化以及實(shí)驗(yàn)運(yùn)行參數(shù)的優(yōu)化提供了參考。
[Abstract]:Solar energy utilization is one of the effective ways to solve the problems of fossil energy shortage, environmental pollution and greenhouse effect in the 21st century because of its unlimited reserves and cleanliness. The energy conversion process combining solar energy with thermochemical reactions not only improves the grade of physical energy to that of chemical energy, but also solves the problems of instability and discontinuity in a single photothermal utilization system. Compared with other hydrogen-making working pairs, ferrite (MFe_2O_4, M=Ni, Co, Cu, Zn, etc.) working pairs are favored by people because of their low pyrolysis temperature, good redox performance and high hydrogen production rate. The development demand of high efficiency and low cost solar energy utilization technology is analyzed. The photothermal-chemical energy transport characteristics of solar thermochemical conversion technology are analyzed. The photothermal transport characteristics in the process of pyrolysis ferrite particles by solar radiation are studied by means of numerical simulation and experimental measurement. Ferrate micro-particles (Ni Fe_2O_4, Cu Fe_2O_4, Mn_ (0.9) Cu_ (0.1) Fe_2O_4) suitable for thermochemical hydrogen production from solar energy at medium and high temperatures were prepared. The purity, particle size and porosity of the prepared particles were obtained by XRD, SEM, and the weight loss curves of Ni Fe_2O_4 and Cu Fe_2O_4 particles at different heating rates were obtained by synchronous thermal analyzer. Based on the weightlessness curve, the thermal decomposition kinetics parameters of Ni Fe_2O_4 and Cu Fe_2O_4 particles were obtained by Flynn-Wall-Ozawa method: apparent activation energy, pre-exponential factor and mechanism function. The measurement error and uncertainty of the experimental system are obtained. The spectral transmission characteristics of ferrite particles in the spectral range of 0.5-2.1 micron are measured by potassium bromide sheeting method. The complex refractive index of ferrite particles is obtained by using Mie theory and KK relation inversion. Planck mean factor method is used to analyze the relationship between the average absorption factor of ferrite particles and temperature.The optical transport model of multi-layer-multi-disk concentrator is established,the design parameters of multi-disk system are corrected,the distribution law of heat flow in the focal plane of solar multi-disk concentrator is analyzed,and the mirror fixation in solar multi-disk concentrator is revealed. The influence mechanism of bolt migration on thermal speckle accumulation was studied. The photothermal transport model of thermochemical reaction flow in the process of pyrolysis of metal oxide particles by solar energy was established by Monte Carlo method and finite volume method. The influence of operating parameters on the thermal performance of the reaction chamber was analyzed, and the influence of solar direct heat flux density and protective gas flow rate on the inner wall temperature of the reactor was obtained. The physical and chemical characteristics of the reactor under different operating conditions (particle size, mass flow rate, protective gas flow rate, temperature, etc.) were studied. The system efficiency and solar-chemical energy under different operating conditions were studied by the second law of thermodynamics, considering the ideal working medium of Ni Fe_2O_4 and Cu Fe_2O_4 for solar thermochemical system. The research results provide a reference for the optimization of solar thermochemical reactor and the optimization of experimental operation parameters.
【學(xué)位授予單位】：哈爾濱工業(yè)大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2016
【分類號(hào)】：TK519;TQ116.2

【相似文獻(xiàn)】

相關(guān)期刊論文 前10條

1 屠萍官;鐵酸鹽包復(fù)膜的實(shí)驗(yàn)研究[J];水處理技術(shù);1992年05期

2 屠萍官;玉浦裕;;用鐵酸鹽包復(fù)法處理含重金屬離子的廢液[J];環(huán)境科學(xué)動(dòng)態(tài);1992年02期

3 ;國(guó)外化工技術(shù)[J];陜西化工;1987年01期

4 王靜,鄧彤,馮亞萍,戴玉杰;鈷基鐵酸鹽的室溫合成和表征[J];光譜學(xué)與光譜分析;2005年08期

5 李磊;顧文秀;吳婷婷;王玉如;鄒路易;;鐵酸鹽材料制備及應(yīng)用進(jìn)展[J];現(xiàn)代化工;2013年02期

6 陳英,程永;利用可重復(fù)使用的鐵酸鹽處理飛塵[J];國(guó)外科技動(dòng)態(tài);1995年06期

7 張春雷，吳通好，，楊洪茂，姜玉子，彭少逸;氧缺位鐵酸鹽的制備及結(jié)構(gòu)與還原行為的研究[J];燃料化學(xué)學(xué)報(bào);1996年01期

8 屠萍官;;對(duì)鐵酸鹽法處理過(guò)程中F離子去除的方法實(shí)驗(yàn)[J];環(huán)境保護(hù);1991年06期

9 王祝然;;加石膏的C_4AF的水化機(jī)理和動(dòng)力學(xué)[J];水泥;1982年06期

10 劉輝,魏雨;鐵酸鹽納米粒子的制備及分散性研究[J];無(wú)機(jī)鹽工業(yè);2005年06期

相關(guān)會(huì)議論文 前1條

1 馬令娟;陳林深;陳誦英;;納米多金屬鐵酸鹽分解CO_2的研究[A];第十一屆全國(guó)青年催化學(xué)術(shù)會(huì)議論文集（上）[C];2007年

相關(guān)博士學(xué)位論文 前4條

1 黃興;聚集輻射熱解鐵酸鹽顆粒過(guò)程光熱特性分析[D];哈爾濱工業(yè)大學(xué);2016年

2 沈昱;鐵酸鹽光催化劑的制備及其降解苯的原位紅外光譜研究[D];大連理工大學(xué);2012年

3 馬令娟;鐵酸鹽的H_2還原和CO_2分解反應(yīng)的研究[D];浙江大學(xué);2008年

4 武崢;鐵酸鹽多鐵材料光伏及催化性能研究[D];中國(guó)地質(zhì)大學(xué)（北京）;2014年

相關(guān)碩士學(xué)位論文 前3條

1 尹龍;納米介孔鐵酸鹽的表面化學(xué)反應(yīng)[D];濟(jì)南大學(xué);2014年

2 韓麗靜;鐵酸鹽（ZnFe_204_、BiFe0_3、LaFe0_3）的合成及在PVC和PP中的阻燃應(yīng)用[D];河北大學(xué);2015年

3 蒯三可;Ce~(3+)摻雜Zn鐵酸鹽磁性納米材料制備及污水處理的應(yīng)用[D];揚(yáng)州大學(xué);2014年

本文編號(hào)：2242137