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拓扑半金属，作为一种独特的拓扑电子态，近年来因其固有的拓扑特性和潜在的器件应用而备受研究关注。体-边界对应是拓扑半金属的一个关键特征，这意味着如果在体相中存在非平庸的能带拓扑，那么在表面会存在受拓扑保护导电状态，即拓扑表面态(topological surface state,TSS)。这一特征使其在电催化研究领域备受关注。本文采用第一性原理计算手段研究了AlB2材料的拓扑性质，并构建(010)表面Al端面和B端面平板模型，计算得到了TSS的位置。研究了AlB2表面吸附特性，发现Al端面氢吸附吉布斯自由能(∆GH*)仅为-0.031 eV，相较于商业电催化析氢(hydrogen evolution reaction,HER)催化剂Pt的-0.08 eV更接近于0，展现出了优异的HER性能。观察了AlB2表面吸附H、OH和H2O后TSS的变化，发现当H吸附时TSS变化最显著，其次是OH吸附，H2O因其电中性和弱的表面吸附对TSS的影响很微弱。并且在吸附前后，由于受拓扑保护TSS依旧存在，仅是能量发生了改变，证实了其在环境中的稳定性。本工作研究结果为不同吸附物对AlB2的TSS的影响提供了系统的认识，为今后相关领域的理论和实验研究铺平了道路，也为拓扑材料的实际应用提供了理论支撑。Topological semimetals have been attracting great research interests due to their intrinsic topological physics and potential devices applications. A key feature for all topological materials is the so-called bulk-boundary correspondence, which means if there is non-trivial band topology in the bulk, then we can expect unique topologically protected conducting states in the edges, i.e., the topological surface state (TSS). Previously the studies for the surface states of topological materials mainly focus on the pristine surfaces, while the topological nodal line semimetal surface states with adsorbates are rarely systematically studied. In this paper, the topological properties of the topological semimetal AlB2 are studied by first-principles calculations, and the TSS position is calculated by constructing the Al- and B-terminated slab models. Observing the topological surface state, it is found that the drumhead-like TSS connects two Dirac nodes with no energy gaps on the node line, and the TSS of the Al end-terminated slab has a smaller energy dispersion than that of the B-terminated slab. The adsorption characteristics of AlB2 (010) surface were studied, and it was found that the Gibbs free energy (∆GH*) for hydrogen adsorption on the surface of Al was only -0.031 eV, demonstrating excellent hydrogen evolution reaction (HER) performance. The changes of TSS after surface adsorption of H, OH and H2O on the surface of AlB2 in aqueous solution environment were observed, as shown in FIG. 1. The TSS change was the most significant when H was adsorbed, followed by OH adsorption. And the influence of H2O on TSS due to its electrical neutrality and weak surface adsorption was very weak, Before and after adsorption, because the topology protection TSS still exists, only the energy changes, which confirms its robust in the environment. The results of this work provide a systematic understanding of the effects of different adsorbents on the TSS of AlB2, pave the way for future theoretical and experimental research in related fields, and also provide theoretical support for the practical application of topological materials.
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Keywords:
- topological semimetal /
- topological surface state /
- surface adsorption
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