等离子体增强金属镁纳米团簇上的分子氢解离
Plasmonic enhancement of molecular hydrogen dissociation on metallic magnesium nanoclusters
摘要：
光驱动等离子体增强金属催化剂上的化学反应是实现高选择性和高效化学转化的有前途的策略。等离子体激元催化剂材料的研究传统上集中在后过渡金属如Au、Ag和Cu上。近年来，人们对一组地球上丰富的元素如Mg的等离子体特性越来越感兴趣，这些元素表现出有趣的氢化化学，在储氢方面具有潜在的应用。本工作采用含时密度泛函紧束缚和密度泛函理论计算方法研究了一组含2057个原子的金属镁纳米团簇的光学、电子和催化性质。我们的研究结果表明，镁纳米团簇能够产生高能量的热电子的能量高达4 eV。通过电子结构分析，我们发现这些超热电子与物理吸附的氢分子的电子态在能量上是一致的，超热电子占据氢分子的电子态可以促进氢的解离反应。我们还发现，逆反应，金属镁上的析氢，可以潜在地促进热电子，但遵循不同的机制。因此，从理论的角度来看，镁纳米团簇显示出非常有前途的行为，其用于光促进储存和释放氢。
英文摘要：
Light-driven plasmonic enhancement of chemical reactions on metal catalysts is a promising strategy to achieve highly selective and efficient chemical transformations. The study of plasmonic catalyst materials has traditionally focused on late transition metals such as Au, Ag, and Cu. In recent years, there has been increasing interest in the plasmonic properties of a set of earth-abundant elements such as Mg, which exhibit interesting hydrogenation chemistry with potential applications in hydrogen storage. This work explores the optical, electronic, and catalytic properties of a set of metallic Mg nanoclusters with up to 2057 atoms using time-dependent density functional tight-binding and density functional theory calculations. Our results show that Mg nanoclusters are able to produce highly energetic hot electrons with energies of up to 4 eV. By electronic structure analysis, we find that these hot electrons energetically align with electronic states of physisorbed molecular hydrogen, occupation of which by hot electrons can promote the hydrogen dissociation reaction. We also find that the reverse reaction, hydrogen evolution on metallic Mg, can potentially be promoted by hot electrons, but following a different mechanism. Thus, from a theoretical perspective, Mg nanoclusters display very promising behaviour for their use in light promoted storage and release of hydrogen.
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