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Hydrogen-related defects and the role of metal additives in the kinetics of complex hydrides: A first-principles study

机译:与氢有关的缺陷和金属添加剂在复杂氢化物动力学中的作用:第一性原理研究

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摘要

We report first-principles studies of hydrogen-related point defects and impurities in LiBH_4 and Li_4BN_3H_(10), two promising materials for hydrogen storage. In both systems, hydrogen vacancies and interstitials are found to be positively or negatively charged, and hence their formation energies are Fermi-level dependent. One can therefore tailor the formation energies of these point defects (hence the kinetics of the systems) by shifting the Fermi level. This can be accomplished by adding appropriate impurities that are electrically active into the systems. We have identified a number of transition-metal impurities that are effective in shifting the Fermi level of LiBH_4 and Li_4BN_3H_(10). A comparison of our calculations with experimental results for the effects of addition of impurities on the kinetics of LiBH_4 and Li_4BN_3H_(10) shows qualitative agreement, providing validation for our interpretation of the results and for our proposed model for enhancement of kinetics.
机译:我们报告了第一原理研究氢相关的点缺陷和LiBH_4和Li_4BN_3H_(10),这两种有希望的储氢材料中的杂质。在这两个系统中,发现氢空位和间隙带正电或负电,因此它们的形成能取决于费米能级。因此,可以通过改变费米能级来调整这些点缺陷的形成能(因此改变系统的动力学)。这可以通过添加适当的对系统具有电活性的杂质来实现。我们已经确定了许多过渡金属杂质,它们可以有效地转移LiBH_4和Li_4BN_3H_(10)的费米能级。我们的计算结果与实验结果对杂质添加对LiBH_4和Li_4BN_3H_(10)动力学的影响的比较显示出定性的一致性,为我们对结果的解释和我们提出的动力学增强模型提供了验证。

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