Npj Comput. Mater.:高熵合金催化剂—吸附能的线性关系
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来自美国能源部国家能源技术实验室的Wissam A. Saidi研究了含氢分子*AHx (A为C或N时,x = 0, 1, 2, 3;A为S时,x = 0, 1, 2;A为O时,x = 0, 1)在高熵合金CoMoFeNiCu表面上吸附能性质。作者使用基于特定吸附质和特定位点的深度学习模型,计算得到了*A和*AHx 的吸附能。研究发现,只有当二者的吸附位点具有相同的对称性时,吸附能才呈现出线性关联,这和纯净金属表面普遍存在的线性关系有着明显的区别。进一步的研究表明,所有吸附构型的平均吸附能之间存在一种局部的线性关系,与吸附位点的对称性无关。虽然这是一种弱形式的线性关联,但仍然会阻碍多步反应的完全优化。局部线性关联的出现需要满足(1)近视原理和(2)吸附能在平均值附近集中分布两个条件。近视原理对于所有电子系统普遍成立,而第二个条件仅适用于高熵合金中含有较强反应活性组分的情形。对于贵金属组分的AgAuCuPdPt高熵合金表面,平均吸附能则并不出现局部线性关联。该研究指出,合金并不总是能够打破线性关系,这为高熵合金在催化领域的应用提高了理论指导。
该文近期发表于npj Computational Materials 8:86(2022),英文标题与摘要如下,点击左下角“阅读原文”可以自由获取论文PDF。
Emergence of local scaling relations in adsorption energies on high-entropy alloys
Wissam A. Saidi
Alloying has been proposed to circumvent scaling relations between the adsorption energies thus allowing for the complete optimization of multistep reactions. Herein the fidelity of scaling rules on high-entropy alloy (HEA) surfaces is assessed focusing on hydrogen-containing molecules, *AHx for A = C and N (x = 0, 1, 2, 3), A = S (x = 0, 1, 2) and A = O (x = 0, 1). Using an adsorbate- and site-specific deep learning model to rapidly compute the adsorption energies on CoMoFeNiCu HEA surfaces, the energies of *AHx and *A are shown to be linearly correlated if *A and *AHx have identical adsorption site symmetry. However, a local linear dependence emerges between the configuration-averaged adsorption energies irrespective of the site symmetry. Although these correlations represent a weaker form of the scaling relationships, they are sufficient to prohibit the optimization of multistep reactions. The underpinning of this behavior is twofold (1) the nearsightedness principle and (2) the narrow distribution of the adsorption energies around the mean-field value. While the nearsightedness is general for all electronic systems, the second criterion applies in HEAs with relatively strong reactive elements. The present findings strongly suggest that alloys may not generally enable the breaking of scaling relationships.
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