Computational modeling of metal–oxide interfaces is challenging due to the large search space of compositions and structures and the complexity of catalyst materials under operating conditions in general.In this work...Computational modeling of metal–oxide interfaces is challenging due to the large search space of compositions and structures and the complexity of catalyst materials under operating conditions in general.In this work,we develop an efficient structure search workflow to discover chemically unique and relevant nanocluster geometries of inverse catalysts and apply it to Zn_(y)O_(x)and In_(y)O_(x)on Cu(111),Pd(111),and Au(111).We show that the workflow is successful in obtaining a large range of chemically distinct structures.Structural geometry trends are identified,including stable motifs such as tripod,rhombus,and pyramidal motifs.Using ab initio thermodynamics,we explore the in situ stability of the structures,including single-atom alloys,at a range of oxygen availabilities.This approach allows us to find trends such as the susceptibility to oxidation of the different systems and the range of stability of different cluster motifs.Our analysis highlights the importance of taking the diversity of sites exposed by metal–oxide interfaces into account in catalyst design studies.展开更多
基金funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement No 754513 and The Aarhus University Research Foundation,the Danish National Research Foundation through the Center of Excellence“InterCat”(grant no.DNRF150)VILLUM FONDEN(grant no.37381).Computational support was provided by the Centre for Scientific Computing Aarhus(CSCAA)at Aarhus University.
文摘Computational modeling of metal–oxide interfaces is challenging due to the large search space of compositions and structures and the complexity of catalyst materials under operating conditions in general.In this work,we develop an efficient structure search workflow to discover chemically unique and relevant nanocluster geometries of inverse catalysts and apply it to Zn_(y)O_(x)and In_(y)O_(x)on Cu(111),Pd(111),and Au(111).We show that the workflow is successful in obtaining a large range of chemically distinct structures.Structural geometry trends are identified,including stable motifs such as tripod,rhombus,and pyramidal motifs.Using ab initio thermodynamics,we explore the in situ stability of the structures,including single-atom alloys,at a range of oxygen availabilities.This approach allows us to find trends such as the susceptibility to oxidation of the different systems and the range of stability of different cluster motifs.Our analysis highlights the importance of taking the diversity of sites exposed by metal–oxide interfaces into account in catalyst design studies.
