Design of interfaces with thermodynamic and kinetic specificity is of great importance for hydrogen storage from both an applied and fundamental perspective. Here, in order to destabilize the metal hydride and protect the dehydrogenated products from oxidizing, a unique core-shell structure of porous Mg(BH₄)₂-based framework with a thin layer (no more than 5 nm) of MgCl₂ additives on the surface, has been proposed and synthesized via a wet-chemical method. The local structure and electronic state of the present complex system are systematically investigated to understand the correlation between the distribution of additives and dehydrogenation property of Mg(BH₄)₂. A significant improvement is achieved for hydrogen desorption with chlorides: initial hydrogen release from MgCl₂ decorated γ-phase Mg(BH₄)₂ particles commences at 100 °C and reaches a maximum of 9.4 wt% at 385 °C. Besides the decreased decomposition temperature, an activation barrier of about 76.4 kJ mol⁻¹ lower than that of Mg(BH₄)₂ without MgCl₂ is obtained. Moreover, MgCl₂ decoration can also prevent the whole decomposed system (both Mg- and B- elements) from oxidizing, which is a necessary condition to reversibility.

中文翻译：

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具有核壳结构的多孔硼氢化镁骨架的添加剂去稳定化

从应用和基础的角度来看，具有热力学和动力学特异性的界面设计对于储氢都非常重要。在这里，为了使金属氢化物不稳定并保护脱氢产物免于氧化，多孔 Mg(BH ₄ ) ₂基骨架的独特核壳结构与薄层（不超过 5 nm）的 MgCl ₂添加剂在表面，已经提出并通过湿化学方法合成。系统地研究了当前复杂系统的局部结构和电子状态，以了解添加剂分布与 Mg(BH ₄ ) ₂脱氢性能之间的相关性. 氯化物对氢的解吸实现了显着改进：从 MgCl ₂装饰的 γ 相 Mg(BH ₄ ) ₂颗粒中释放的初始氢在 100 °C 开始，并在 385 °C 时达到最大 9.4 wt%。除了降低的分解温度外，还获得了比不含 MgCl ₂的 Mg(BH ₄ ) ₂的活化能垒低约 76.4 kJ mol ^-1的活化能垒。此外，MgCl ₂修饰还可以防止整个分解系统（包括Mg-和B-元素）氧化，这是可逆性的必要条件。