發(fā)布時間：2018-09-14 08:29

【摘要】：太陽能利用以其儲量無限性、開發(fā)利用清潔性,成為21世紀解決化石能源短缺、環(huán)境污染和溫室效應等問題的有效途徑之一。太陽能高溫熱化學轉(zhuǎn)換是通過聚光產(chǎn)生高溫熱能來驅(qū)動熱化學反應,將所聚集的太陽能轉(zhuǎn)化為碳氫燃料的化學能,并在制氫、溫室氣體減排等領域得到廣泛的研究與應用。太陽能與熱化學反應相結合的能量轉(zhuǎn)換過程不僅使其由物理能品位提升到化學能品位,而且可以將太陽能存儲為解決單獨光熱利用系統(tǒng)不穩(wěn)定、不連續(xù)等問題,有效提高太陽能熱利用系統(tǒng)的效率。相比于其他制氫工質(zhì)對,鐵酸鹽(MFe_2O_4,M=Ni,Co,Cu,Zn等)工質(zhì)對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。本文以兩步熱化學循環(huán)制氫為應用背景,結合實際應用過程中對太陽能高效低成本利用技術的發(fā)展需求,分析了太陽能熱化學轉(zhuǎn)換技術中光-熱-化學能輸運特性,采用數(shù)值模擬與實驗測量相結合的手段研究了聚集太陽輻射熱解鐵酸鹽顆粒過程中光熱傳輸特性。主要的研究內(nèi)容如下:采用化學共沉淀法制備了適用于中高溫太陽能熱化學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顆粒的熱分解動力學三參數(shù):表觀活化能、指前因子和機理函數(shù)。搭建了用于能源材料光譜輻射物性測量的實驗裝置,通過中國計量院的標準樣片實驗數(shù)據(jù)獲得了實驗系統(tǒng)的測量誤差以及測量不確定度。采用溴化鉀壓片法測量了鐵酸鹽微顆粒在光譜區(qū)間0.5-2.1μm的光譜透過特性;運用Mie理論和KK關系式反演獲得了鐵酸鹽粒子的復折射率與光譜的變化關系;基于計算得到復折射率,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系。建立了多層-多碟聚光器的光輸運模型,校正了多碟系統(tǒng)設計參數(shù)并分析了太陽能多碟聚光系統(tǒng)焦平面熱流的分布規(guī)律,揭示了太陽能多碟聚光系統(tǒng)中反射鏡固定螺栓遷移對聚集熱流散斑的影響機理。采用蒙特卡洛法與有限體積法建立太陽能熱裂解金屬氧化物顆粒過程中熱化學反應流的光熱輸運模型,分析了Ni Fe_2O_4反應顆粒粒徑、質(zhì)量流量、保護氣體流速以及溫度等對反應器內(nèi)溫度場、流場分布以及反應顆粒轉(zhuǎn)化率的影響;研制了腔式太陽能熱化學反應器,分析了運行參數(shù)對反應腔熱性能的影響,獲得了太陽直射熱流密度以及保護氣體流量對反應器內(nèi)壁面溫度的影響規(guī)律。采用?理論并結合UDF技術數(shù)值分析了太陽能熱化學反應器在不同工況參數(shù)(反應顆粒粒徑、質(zhì)量流量、保護氣體流速以及溫度等)時物理?和化學?的分布特性;考慮理想Ni Fe_2O_4和Cu Fe_2O_4工質(zhì)對太陽能熱化學系統(tǒng),采用熱力學第二定律研究了不同工況參數(shù)對系統(tǒng)效率以及太陽能-化學能轉(zhuǎn)化效率的影響;研究結果為太陽能熱化學反應器的優(yōu)化以及實驗運行參數(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.
【學位授予單位】：哈爾濱工業(yè)大學
【學位級別】：博士
【學位授予年份】：2016
【分類號】：TK519;TQ116.2

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