Xu Qiunan, Li Guowei, Zhang Yang, Yang Qun, Sun Yan, Felser Claudia
Max Planck Institute for Chemical Physics of Solids, 01187 Dresden, Germany.
Center for Nanoscale Systems, Faculty of Arts and Sciences, Harvard University, 11 Oxford Street, LISE 308, Cambridge, Massachusetts 02138, United States.
ACS Catal. 2020 May 1;10(9):5042-5048. doi: 10.1021/acscatal.9b05539. Epub 2020 Apr 3.
The vital role of electrocatalysts in determining the efficiency of renewable energy conversion inspired the uncovering of the relation between the catalytic efficiency and electronic structure, in which the volcano-type plot based on adsorption energies and d-band model has achieved great success. At the same time, catalysts with nontrivial topological electronic structures have received considerable attention because of their robust topological surface states and high-mobility electrons, which favor the electrons transfer processes in the heterogeneous catalysis reactions. Under the guidance of this theory, excellent catalysts were reported among topological materials. Inspired by the current development of catalyst and topological materials, we tried to extract a pure intrinsic physical parameter, projected Berry phase (PBP), that only depends on the bulk electronic structure. Applying this parameter to the well-known nonmagnetic transition-metal electrocatalysts, we found a linear relationship between PBP and catalytic efficiency of hydrogen evolution reaction (HER) after considering the symmetry constraint. This can be used as a descriptor for the prediction and designing of promising catalysts for HER, which is realized experimentally in PtCu nanostructures. This work illustrates the importance of the pure bulk band structure effect on electrochemical activities and implies an effective way to understand the mechanism of HER catalysts.
电催化剂在决定可再生能源转换效率方面的关键作用激发了人们对催化效率与电子结构之间关系的探索，其中基于吸附能和d带模型的火山型曲线取得了巨大成功。与此同时，具有非平凡拓扑电子结构的催化剂因其稳健的拓扑表面态和高迁移率电子而受到广泛关注，这有利于多相催化反应中的电子转移过程。在该理论的指导下，拓扑材料中报道了优异的催化剂。受当前催化剂和拓扑材料发展的启发，我们试图提取一个仅依赖于体电子结构的纯本征物理参数——投影贝里相位（PBP）。将该参数应用于著名的非磁性过渡金属电催化剂，在考虑对称性约束后，我们发现PBP与析氢反应（HER）的催化效率之间存在线性关系。这可作为预测和设计有前景的HER催化剂的描述符，并在PtCu纳米结构中通过实验得以实现。这项工作说明了纯体带结构效应在电化学活性方面的重要性，并暗示了一种理解HER催化剂机理的有效方法。
