Hydrogen spillover mechanism on a Pd-doped Mg surface as revealed by ab initio density functional calculation
Hydrogen spillover mechanism on a Pd-doped Mg surface as revealed by ab initio density functional calculation
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DOI：
10.1021/ja0722776
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发表时间：
2007-08-22
影响因子：
15
通讯作者：
Lu, G. Q.
中科院分区：
文献类型：
--
作者：
Du, A. J.;Smith, Sean C.;Lu, G. Q.
镁的氢化动力学较慢，阻碍了其在移动的储氢方面的应用。我们证明，通过从头计算密度泛函理论（DFT）计算，反应路径可以大大修改通过添加过渡金属催化剂。与Ti掺杂相比，Pd掺杂将导致分子氢的解离和原子H在Mg表面上的扩散的非常小的活化势垒。这一新的计算发现首次通过从头算模拟支持了所提出的氢溢出机制，该机制用于合理化实验观察到的Pd封端的Mg材料的快速氢化动力学。
The hydrogenation kinetics of Mg is slow, impeding its application for mobile hydrogen storage. We demonstrate by ab initio density functional theory (DFT) calculations that the reaction path can be greatly modified by adding transition metal catalysts. Contrasting with Ti doping, a Pd dopant will result in a very small activation barrier for both dissociation of molecular hydrogen and diffusion of atomic H on the Mg surface. This new computational finding supportsfor the first time by ab initio simulationthe proposed hydrogen spillover mechanism for rationalizing experimentally observed fast hydrogenation kinetics for Pd-capped Mg materials.