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混合導體透氧膜還原性氣氛下分解水制氫研究

發(fā)布時間:2018-03-25 05:25

  本文選題:鈣鈦礦 切入點:混合導體透氧膜 出處:《昆明理工大學》2017年碩士論文


【摘要】:近些年來,能源形勢和環(huán)境問題日趨惡化,這迫使我們需要尋找新的替代能源。其中氫能有著零污染、熱值高等優(yōu)點被世界各國所推崇。制取氫氣的方法多種多樣,其中研究較多要屬熱化學分解水制氫。熱化學分解水制氫經歷了化學鏈制氫到如今的利用混合導體透氧膜材料分解水制氫的過程。在經過大量查閱文獻后,本論文選擇了在還原性氣氛下結構穩(wěn)定的三種鈣鈦礦氧化物(La0.9Ca0.1FeO3-δ、BaFe0.9Zr0.1O3-δ以及La0.6Sr0.4Coo.8Gao.2O3-δ)作為研究對象,分別對這三種混合導體透氧膜氧材料進行了各種表征與透氧性能評價;最后通過XRD、Raman、SEM等手段研究了在還原氣氛下它們的熱化學結構穩(wěn)定性以及分解水制氫性能。本文中 Lao.9Cao.1FeO3-δ(LCF-91)、BaFeo.9Zro.1O3-δ(BFZ-91)以及Lao.6Sr0.4Co0.8Gao.2O3-δ(LSCG-6482)鈣鈦礦透氧膜材料是通過溶膠凝膠法制備合成的。為了探究這幾種混合導體透氧膜材料的物相組成、形成過程中熱量與質量變化以及氧化還原性能,本文采用了 XRD、TG-DSC和H2-TPR等表征手段對它們進行了分析和表征,同時還進行了 CH4-TPR、CO-TPR實驗對這幾種膜材料的活性進行了評價。隨后將混合導體透氧膜與膜反應器耦合并在反應器內進行了透氧性能與產氫性能的評價。在這三種膜材料的透氧實驗中,發(fā)現LCF-91、BFZ-91以及LSCG-6482在900℃時的氧滲透性較好,且最高透氧量分別為1.65、2.28和3.06×10-8mol·s-1·cm-2。此外,還對透氧實驗后的三種膜材料進行了 XRD、SEM表征分析,實驗結果表明LCF-91、BFZ-91以及LSCG-6482透氧膜材料反應前后結構均勻致密,熱化學穩(wěn)定性良好。在還原性氣氛下分解水制氫實驗中,分別對混合導體透氧膜材料LCF-91、BFZ-91以及LSCG-6482的氧化側產氫以及還原側產物進行了評價分析,發(fā)現LCF-91、BFZ-91以及LSCG-6482膜分解水制氫在還原性氣氛下均容易進行,產氫性能良好。我們還對其反應后膜材料進行XRD物相、SEM以及拉曼圖譜分析,分析結果表明混合導體透氧膜材料LCF-91、BFZ-91以及LSCG-6482分解水制氫后結構穩(wěn)定性較好。
[Abstract]:In recent years, the energy situation and environmental problems are getting worse and worse, which forces us to find new alternative energy. Hydrogen energy has the advantages of zero pollution, high calorific value and so on. Among them, the research mainly belongs to thermochemical decomposition of water to produce hydrogen. Thermochemical decomposition of water for hydrogen production has gone through the process of chemical chain hydrogen production until now, using mixed conductor oxygen permeable membrane materials to decompose water to produce hydrogen. In this thesis, three kinds of perovskite oxides, La0.9Ca0.1FeO3- 未 BaFe0.9Zr0.1O3- 未 and La0.6Sr0.4Coo.8Gao.2O3- 未, which have stable structure in reductive atmosphere, are selected as the research objects. Finally, the stability of their thermochemical structures and the properties of hydrogen production from water were studied by means of XRDX Ramanum SEM. In this paper, Lao.9Cao.1FeO3- 未 LSCG-6482) perovskite perovskite membrane materials were prepared by sol-gel method, BaFeo.9Zro.1O3- 未 (BFZ-91) and Lao.6Sr0.4Co0.8Gao.2O3- 未 (LSCG-6482) perovskite perovskite membrane materials were prepared by sol-gel method. To explore the phase composition of these mixed conductor oxygen permeable membrane materials, The heat and mass changes and redox properties during the formation were analyzed and characterized by means of XRDX TG-DSC and H2-TPR. At the same time, the activity of these membrane materials was evaluated by CH4-TPR-CO-TPR experiment. Then the mixed conductor oxygen permeable membrane was coupled with the membrane reactor, and the oxygen permeability and hydrogen production performance were evaluated in the reactor. In the oxygen permeation experiment of materials, It was found that the oxygen permeability of LCF-91 and LSCG-6482 was better at 900 鈩,

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