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Hydrogen desorption kinetics in transition metal modified NaAlH_4

机译:过渡金属修饰的NaAlH_4中的氢解吸动力学

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The compound NaAlH_4 has been proposed as a viable hydrogen storage media capable of supplying hydrogen at moderate temperatures and at rates required for fuel cell applications. A number of researchers have subsequently verified and enhanced the rate of dehydrogenation in this system using combined transition metal catalytic additions along with different methods of their introduction into the NaAlH_4 compound. The most potent catalytic addition identified thus far is TiCl_3 added through ball milling, however, ZrCl_3 and other transition metal chlorides have also been found useful. To this date, the role of the catalysts are still unknown as well as their disposition within the NaAlH_4 compound. This investigation has sought to identify the extent catalytic dehydrogenation reaction rate of a number of transition metal additions to NaAlH_4 at 120 deg C. Two mol percent catalysts were added, primarily as chlorides, in a number of valance states. High energy ball mill attrition of the catalyst and the alanate were made with optimum milling times determined. Comparison of dehydrogenation rates with ion radius has shown an optimum catalyst ion radius ratio to be readily identifiable as being midway between that of Al(III) and Na(I). Cation valance, while an important factor in hydrogen discharge kinetics, was shown not to be the primary contributing factor for catalytic activity.
机译:已经提出了化合物NaAlH_4作为可行的氢存储介质,其能够在中等温度下以燃料电池应用所需的速率供应氢。随后,许多研究人员通过结合使用过渡金属催化添加物以及将其引入NaAlH_4化合物的不同方法,验证并提高了该系统中的脱氢速率。迄今为止,确定的最有效的催化添加是通过球磨添加的TiCl_3,但是,还发现ZrCl_3和其他过渡金属氯化物是有用的。迄今为止,催化剂的作用及其在NaAlH_4化合物中的位置仍然未知。这项研究试图确定在120℃下向NaAlH_4中添加的多种过渡金属的催化脱氢反应速率的程度。以许多价态添加了2摩尔%的催化剂,主要是作为氯化物。用确定的最佳研磨时间进行催化剂和丙氨酸的高能球磨机磨耗。脱氢速率与离子半径的比较表明,可以容易地确定最佳催化剂离子半径比为Al(III)和Na(I)的中间值。阳离子化合价虽然是氢放电动力学的重要因素,但并不是催化活性的主要贡献因素。

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