Electronic structure factors and the importance of adsorbate effects in chemisorption on surface alloys

作     者：Shikha Saini Joakim Halldin Stenlid Frank Abild-Pedersen 

作者机构：SUNCAT Center for Interface Science and CatalysisDepartment of Chemical EngineeringStanford University443 Via OrtegaStanfordCA94305USA SUNCAT Center for Interface Science and CatalysisSLAC National Accelerator Laboratory2575 Sand Hill RoadMenlo ParkCA94025USA 

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：1560-1571页

核心收录：

学科分类：08[工学] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：J.H.S.gratefully acknowledge funding via the Knut and Alice Wallenberg foundation(grant no.2019.0586) We thank Dr.Johannes Voss,Dr.Karun Kumar Rao and Dr.Benjamin Comer for fruitful discussions and acknowledge computational support from the National Energy Research Scientific Computing Center(computer time allocation m2997),a DOE Office of Science User Facility supported by the Office of Science of the U.S.Department of Energy under Contract No.DE-AC02-05CH11231 

主　　题：alloys corrosion chemisorption 

摘      要：The chemisorption energy is an integral aspect of surface chemistry,central to numerous fields such as catalysis,corrosion,and ***-structure-based methods such as the Newns-Anderson model are therefore of great importance in guiding the engineering of material surfaces with optimal ***,existing methods are inadequate for interpreting complex,multi-metallic ***,we introduce a physics-based chemisorption model for alloyed transition metal surfaces employing primarily metal d-band properties that accounts for perturbations in both the substrate and adsorbate electronic states upon ***,we show that adsorbate-induced changes in the adsorption site interact with its chemical environment leading to a second-order response in chemisorption energy with the d-filling of the neighboring *** demonstrate the robustness of the model on a wide range of transition metal alloys with O,N,CH,and Li adsorbates yielding a mean absolute error of 0.13 eV versus density functional theory reference chemisorption energies.