Efficient hydrogen evolution reaction due to topological polarization
Efficient hydrogen evolution reaction due to topological polarization
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DOI：
10.1103/physrevb.106.165120
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发表时间：
2022-07
影响因子：
3.7
通讯作者：
M. Jiang;G. Guo;M. Hirayama;T. Yu;T. Nomoto;R. Arita
中科院分区：
文献类型：
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作者：
M. Jiang;G. Guo;M. Hirayama;T. Yu;T. Nomoto;R. Arita
携带拓扑表面态（TSS）的材料为析氢反应（HER）提供了一个迷人的平台。基于a3b （A = Ni, Pd, Pt; B = Si, Ge, Sn）的系统第一性原理计算，我们提出以Zak相为特征的拓扑电极化对于设计高效的HER催化剂至关重要。对于a3b，我们证明了Zak相在整个（111）投影布里渊区具有非平凡的π值，这导致了表面的量子化极化电荷。在那里，取决于吸附位置，氢原子(H)与TSS杂化而不是与体态杂化。当杂化作用介于共价键和离子键之间时，H态在能谱上定位，吸附H引起的吉布斯自由能变化（∆G）变小。也就是说，H态和底物之间的相互作用变得相当弱，这对HER是非常有利的。值得注意的是，我们发现Pt 3sn和Pd 3sn的∆G分别仅为-0.066和-0.092 eV，几乎是Pt值的一半。
Materials carrying topological surface states (TSS) provide a fascinating platform for the hydrogen evolution reaction (HER). Based on systematic first-principles calculations for A 3 B ( A = Ni, Pd, Pt; B = Si, Ge, Sn), we propose that topological electric polarization characterized by the Zak phase can be crucial to designing efficient catalysts for the HER. For A 3 B , we show that the Zak phase takes a nontrivial value of π in the whole (111) projected Brillouin zone, which causes quantized electric polarization charge at the surface. There, depending on the adsorption sites, the hydrogen (H) atom hybridizes with the TSS rather than with the bulk states. When the hybridization has an intermediate character between the covalent and ionic bond, the H states are localized in the energy spectrum, and the change in the Gibbs free energy (∆ G ) due to the H adsorption becomes small. Namely, the interaction between the H states and the substrate becomes considerably weak, which is a highly favorable situation for the HER. Notably, we show that ∆ G for Pt 3 Sn and Pd 3 Sn are just -0.066 and -0.092 eV, respectively, which are almost half of the value of Pt.