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铝/硼氢化钠可控制体系的性能及反应机理研究
马广璐
学位类型硕士
导师王平 ; 戴洪斌
2012
学位授予单位中国科学院金属研究所
学位授予地点北京
学位专业材料学
关键词储氢材料 可控制氢 硼氢化钠 Hydrogen Storage Material Controlled Hydrogen Generation Aluminum Sodium Borohydride
摘要"摘 要

        氢能是一种理想的清洁能源载体,具有许多优点,但是它的存储/制备是推动其规模化商业应用的关键环节。铝(Al)/水(H2O)反应可控制氢作为一种安全环保的储氢/制氢技术,其关键在于破坏或抑制铝表面固有的氧化膜或原位再生的钝化膜;另外,与其它化学储氢/制氢体系(例如,硼氢化钠(NaBH4)和氨基硼烷(NH3BH3)等)相比,Al/H2O制氢体系的储氢密度较低。本论文围绕以上二个科学/技术问题,开展了以下工作:
(1)         针对常规Al/H2O反应制氢体系需高浓度氢氧化钠(NaOH)的问题,采用锡酸钠(Na2SnO3)和NaOH混合促进剂,分别构建了Al/NaOH-Na2SnO3-H2O制氢体系和Al-NaOH-Na2SnO3/H2O制氢体系,显著加速了Al/H2O反应的动力学,降低了反应所需碱的浓度,并对该制氢体系性能的反应机理进行了分析。
(2)         针对Al/H2O反应制氢体系储氢密度低的问题,构建了新型双燃料制氢体系:Al-NaBH4(固)-NaOH/氯化钴(CoCl2)水溶液和NaBH4-NaOH-H2O/Al-催化剂。通过调节固、液两相的接触和分离可以方便地控制产氢。研究表明:NaBH4水解反应和Al/H2O反应存在相互促进的反应机理,因此,显著提高了双重燃料制氢体系的反应动力学,并且提高了Al/H2O制氢体系的储氢密度,降低了NaBH4制氢体系的成本。该研究构建的新型高效可控的制氢体系,为研发实用型移动或便携式制氢装置提供了实验/理论基础。"
其他摘要"
Abstract
Hydrogen is an ideal clean energy carrier with many an advantage. However, hydrogen storage/generation has been the key point of commercial applications of hydrogen energy. Aluminum(Al)/water(H2O) reaction as a controlled source of hydrogen is security and environmentally friendly, and its key technical challenge is to disrupt the oxide layer or to inhibit the formation of a coherent and adherent passivation layer on the surface of Al. Furthermore, the hydrogen density of Al/H2O reaction system is lower than chemical hydrides hydrolysis system, such as sodium borohydride (NaBH4) and ammonia borohydride (NH3BH3). In the present study, we focus on the two problems mentioned above.

(1)   For the sake of decreasing the necessary sodium hydroxide (NaOH) concentration of Al/H2O reaction syetem, two hydrogen generation systems using combination of NaOH and sodium stannate(Na2SnO3)have been demonstrated, respectively. One system is composed of Al/Na2SnO3-NaOH-H2O; the other is composed of Al-NaOH-Na2SnO3/H2O. The combined usage of NaOH and Na2SnO3 can dramatically improve the hydrogen generation kinetics of the Al/H2O systems. Besides, the addition of a small amount of Na2SnO3 caused a significantly lowered requirement of the quantity of NaOH promoter. A preliminary study has been carried out to gain mechanistic understanding of these interesting observations.
(2)   For the sake of improvement of the hydrogen density of Al/H2O reaction syetem, two hydrogen generation systems have been demonstrated, respectively. One of these systems was composed of Al-NaBH4-NaOH solid mixture/cobalt chloride(CoCl2) aqueous solution; the other system was composed of NaBH4-NaOH-H2O/solid powder mixture of Al powder and catalyst. In thess systems, hydrogen generation can be readily controlled by regulating the solutions to contact with or leave the solid mixture. In comparison with the conventional single fuel systems, the NaBH4 -Al/H2O system exhibited a series of property advantages, such as higher HG rate, increased fuel conversion, higher hydrogen density and reduced H2 production cost than NaBH4 hydrolysis system. Fundamentally, the improvements on the HG properties originate from the mutual-promoting mechanism between the hydrolysis reaction of NaBH4 and the Al/H2O reaction. In this regard, the studies may lay a basis for designing practical mobile/ portable hydrogen generator."
文献类型学位论文
条目标识符http://ir.imr.ac.cn/handle/321006/64524
专题中国科学院金属研究所
推荐引用方式
GB/T 7714
马广璐. 铝/硼氢化钠可控制体系的性能及反应机理研究[D]. 北京. 中国科学院金属研究所,2012.
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