{"title":"Reactant-induced dynamics of lithium imide surfaces during the ammonia decomposition process","authors":"Manyi Yang, Umberto Raucci, Michele Parrinello","doi":"10.1038/s41929-023-01006-2","DOIUrl":null,"url":null,"abstract":"Ammonia decomposition on lithium imide surfaces has been intensively investigated owing to its potential role in a sustainable hydrogen-based economy. Here, through advanced molecular dynamics simulations of ab initio accuracy, we show that the surface structure of the catalyst changes on exposure to the reactants and a dynamic state is activated. It is this highly fluctuating state that is responsible for catalysis and not a well-defined static catalytic centre. In this activated environment, a series of reactions that eventually leads to the release of N2 and H2 molecules becomes possible. Once the flow of reagent is terminated, the imide surface returns to its pristine state. We suggest that by properly engineering this dynamic interfacial state one can design improved catalytic systems. The common static description of catalysts during turnover has often been challenged, but their specific nature under such conditions remains elusive. Now complex simulations reveal that ammonia decomposition on LiNH surfaces is catalysed by a highly dynamic, liquid-like interface that reversibly forms under operation.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"6 9","pages":"829-836"},"PeriodicalIF":42.8000,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.nature.com/articles/s41929-023-01006-2","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Ammonia decomposition on lithium imide surfaces has been intensively investigated owing to its potential role in a sustainable hydrogen-based economy. Here, through advanced molecular dynamics simulations of ab initio accuracy, we show that the surface structure of the catalyst changes on exposure to the reactants and a dynamic state is activated. It is this highly fluctuating state that is responsible for catalysis and not a well-defined static catalytic centre. In this activated environment, a series of reactions that eventually leads to the release of N2 and H2 molecules becomes possible. Once the flow of reagent is terminated, the imide surface returns to its pristine state. We suggest that by properly engineering this dynamic interfacial state one can design improved catalytic systems. The common static description of catalysts during turnover has often been challenged, but their specific nature under such conditions remains elusive. Now complex simulations reveal that ammonia decomposition on LiNH surfaces is catalysed by a highly dynamic, liquid-like interface that reversibly forms under operation.
期刊介绍:
Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry.
Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.