{"title":"Al2O3对Fe/γ-Al2O3合成氨Fe催化剂可能有强烈的促进作用","authors":"Jianfu Chen, Ye Chen, Huihui Liu* and P. Hu*, ","doi":"10.1021/acscatal.5c03006","DOIUrl":null,"url":null,"abstract":"<p >Al<sub>2</sub>O<sub>3</sub> is a critical component in Fe-based catalysts for ammonia synthesis, yet its precise promotional role remains elusive. In this work, we employ density functional theory (DFT) and molecular dynamics (MD) simulations to investigate the catalytic behavior of Fe surfaces supported on γ-Al<sub>2</sub>O<sub>3</sub>, the most common phase of Al<sub>2</sub>O<sub>3</sub> used as a support. A series of Fe(110)/γ-Al<sub>2</sub>O<sub>3</sub> models with varying Fe layer thicknesses are constructed, in which the Fe(110) facet is typically the least active among Fe surfaces. Reaction energies and activation barriers are computed for each system, followed by microkinetic simulations based on the calculated energetics. The results reveal a pronounced promotional effect of γ-Al<sub>2</sub>O<sub>3</sub>: Its interaction with Fe(110) significantly lowers the barrier for N<sub>2</sub> dissociative adsorption, elevating the predicted catalytic activity to a level comparable with that of Fe(111), the most active Fe surface. Structural analysis further shows that monolayer Fe(110)/γ-Al<sub>2</sub>O<sub>3</sub> closely resembles the geometry of stepped Fe surfaces. As the number of Fe layers increases, the structural distortion induced by γ-Al<sub>2</sub>O<sub>3</sub> diminishes, and the system gradually reverts to the characteristics of pristine Fe(110).</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"15 15","pages":"13366–13376"},"PeriodicalIF":13.1000,"publicationDate":"2025-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Possible Strong Promotional Effect of Al2O3 on Fe Catalysts for Ammonia Synthesis via Fe/γ-Al2O3\",\"authors\":\"Jianfu Chen, Ye Chen, Huihui Liu* and P. Hu*, \",\"doi\":\"10.1021/acscatal.5c03006\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Al<sub>2</sub>O<sub>3</sub> is a critical component in Fe-based catalysts for ammonia synthesis, yet its precise promotional role remains elusive. In this work, we employ density functional theory (DFT) and molecular dynamics (MD) simulations to investigate the catalytic behavior of Fe surfaces supported on γ-Al<sub>2</sub>O<sub>3</sub>, the most common phase of Al<sub>2</sub>O<sub>3</sub> used as a support. A series of Fe(110)/γ-Al<sub>2</sub>O<sub>3</sub> models with varying Fe layer thicknesses are constructed, in which the Fe(110) facet is typically the least active among Fe surfaces. Reaction energies and activation barriers are computed for each system, followed by microkinetic simulations based on the calculated energetics. The results reveal a pronounced promotional effect of γ-Al<sub>2</sub>O<sub>3</sub>: Its interaction with Fe(110) significantly lowers the barrier for N<sub>2</sub> dissociative adsorption, elevating the predicted catalytic activity to a level comparable with that of Fe(111), the most active Fe surface. Structural analysis further shows that monolayer Fe(110)/γ-Al<sub>2</sub>O<sub>3</sub> closely resembles the geometry of stepped Fe surfaces. As the number of Fe layers increases, the structural distortion induced by γ-Al<sub>2</sub>O<sub>3</sub> diminishes, and the system gradually reverts to the characteristics of pristine Fe(110).</p>\",\"PeriodicalId\":9,\"journal\":{\"name\":\"ACS Catalysis \",\"volume\":\"15 15\",\"pages\":\"13366–13376\"},\"PeriodicalIF\":13.1000,\"publicationDate\":\"2025-07-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Catalysis \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acscatal.5c03006\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acscatal.5c03006","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Possible Strong Promotional Effect of Al2O3 on Fe Catalysts for Ammonia Synthesis via Fe/γ-Al2O3
Al2O3 is a critical component in Fe-based catalysts for ammonia synthesis, yet its precise promotional role remains elusive. In this work, we employ density functional theory (DFT) and molecular dynamics (MD) simulations to investigate the catalytic behavior of Fe surfaces supported on γ-Al2O3, the most common phase of Al2O3 used as a support. A series of Fe(110)/γ-Al2O3 models with varying Fe layer thicknesses are constructed, in which the Fe(110) facet is typically the least active among Fe surfaces. Reaction energies and activation barriers are computed for each system, followed by microkinetic simulations based on the calculated energetics. The results reveal a pronounced promotional effect of γ-Al2O3: Its interaction with Fe(110) significantly lowers the barrier for N2 dissociative adsorption, elevating the predicted catalytic activity to a level comparable with that of Fe(111), the most active Fe surface. Structural analysis further shows that monolayer Fe(110)/γ-Al2O3 closely resembles the geometry of stepped Fe surfaces. As the number of Fe layers increases, the structural distortion induced by γ-Al2O3 diminishes, and the system gradually reverts to the characteristics of pristine Fe(110).
期刊介绍：
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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