Emergence of local scaling relations in adsorption energies on high-entropy alloys

作     者：Wissam A.Saidi 

作者机构：National Energy Technology LaboratoryUnited States Department of EnergyPittsburghPA15236USA Department of Mechanical Engineering and Materials ScienceUniversity of PittsburghPittsburghPA15261USA 

出 版 物：《npj Computational Materials》 (计算材料学（英文）)

年 卷 期：2022年第8卷第1期

页      面：815-821页

核心收录：

学科分类：0710[理学-生物学] 08[工学] 0805[工学-材料科学与工程（可授工学、理学学位）] 080502[工学-材料学] 0714[理学-统计学（可授理学、经济学学位）] 0701[理学-数学] 0812[工学-计算机科学与技术（可授工学、理学学位）] 

基　　金：Pittsburgh Center for Research Computing U.S. Government CRC Health Group, CRC University of Pittsburgh, (DE-AC02-06CH11357) 

主　　题：alloys alloy adsorption 

摘      要：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,^(*)AH_(x) 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 ^(*)AH_(x) and ^(*)A are shown to be linearly correlated if ^(*)A and ^(*)AH_(x) 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.