混合导体透氧膜还原性气氛下分解水制氢研究

发布时间：2018-03-25 05:25

  本文选题：钙钛矿　切入点：混合导体透氧膜　出处：《昆明理工大学》2017年硕士论文

【摘要】：近些年来,能源形势和环境问题日趋恶化,这迫使我们需要寻找新的替代能源。其中氢能有着零污染、热值高等优点被世界各国所推崇。制取氢气的方法多种多样,其中研究较多要属热化学分解水制氢。热化学分解水制氢经历了化学链制氢到如今的利用混合导体透氧膜材料分解水制氢的过程。在经过大量查阅文献后,本论文选择了在还原性气氛下结构稳定的三种钙钛矿氧化物(La0.9Ca0.1FeO3-δ、BaFe0.9Zr0.1O3-δ以及La0.6Sr0.4Coo.8Gao.2O3-δ)作为研究对象,分别对这三种混合导体透氧膜氧材料进行了各种表征与透氧性能评价;最后通过XRD、Raman、SEM等手段研究了在还原气氛下它们的热化学结构稳定性以及分解水制氢性能。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)钙钛矿透氧膜材料是通过溶胶凝胶法制备合成的。为了探究这几种混合导体透氧膜材料的物相组成、形成过程中热量与质量变化以及氧化还原性能,本文采用了 XRD、TG-DSC和H2-TPR等表征手段对它们进行了分析和表征,同时还进行了 CH4-TPR、CO-TPR实验对这几种膜材料的活性进行了评价。随后将混合导体透氧膜与膜反应器耦合并在反应器内进行了透氧性能与产氢性能的评价。在这三种膜材料的透氧实验中,发现LCF-91、BFZ-91以及LSCG-6482在900℃时的氧渗透性较好,且最高透氧量分别为1.65、2.28和3.06×10-8mol·s-1·cm-2。此外,还对透氧实验后的三种膜材料进行了 XRD、SEM表征分析,实验结果表明LCF-91、BFZ-91以及LSCG-6482透氧膜材料反应前后结构均匀致密,热化学稳定性良好。在还原性气氛下分解水制氢实验中,分别对混合导体透氧膜材料LCF-91、BFZ-91以及LSCG-6482的氧化侧产氢以及还原侧产物进行了评价分析,发现LCF-91、BFZ-91以及LSCG-6482膜分解水制氢在还原性气氛下均容易进行,产氢性能良好。我们还对其反应后膜材料进行XRD物相、SEM以及拉曼图谱分析,分析结果表明混合导体透氧膜材料LCF-91、BFZ-91以及LSCG-6482分解水制氢后结构稳定性较好。
[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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