C. Giudici, G. Contaldo, M. Ferri, L. Pratali Maffei, M. Bracconi, M. Pelucchi and M. Maestri
{"title":"Understanding heterogeneous growth mechanisms at graphene edges: a theoretical study on acetylene deposition and mechanistic analysis†","authors":"C. Giudici, G. Contaldo, M. Ferri, L. Pratali Maffei, M. Bracconi, M. Pelucchi and M. Maestri","doi":"10.1039/D4RE00096J","DOIUrl":null,"url":null,"abstract":"<p >This study aims to bridge significant knowledge gaps in the understanding of graphene growth mechanisms. We enhance current kinetic models through a detailed investigation of C<small><sub>2</sub></small>H<small><sub>2</sub></small> deposition processes on solid graphene surfaces. These processes represent key elementary reaction steps in the complex heterogeneous network responsible for pyrocarbon formation during chemical vapor deposition and infiltration processes. Unlike previous methodologies that relied on analogies with gas-phase systems, our research meticulously explored the actual system, providing a comprehensive overview of the reactions involved in graphene growth at both armchair and zigzag edges. Utilizing transition state theory, we calculate accurate, temperature-dependent rate constants for all elementary reactions in graphene edge growth. This sheds light on the mechanisms and kinetics of pyrocarbon growth, including the potential for structural defect formation. Findings are compared with analogous gas-phase reactions responsible for soot particle formation, assessing the impact of surface interactions. A lumping technique is applied to reduce the complexity of species and reactions while preserving the accuracy of the chemical description. As such, this approach offers valuable insights into relevant pathways paving the way towards a deep understanding of the chemistry of the pyrolysis of hydrocarbons aiming to produce nanomaterials with targeted properties.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.4000,"publicationDate":"2024-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/re/d4re00096j?page=search","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Reaction Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/re/d4re00096j","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
This study aims to bridge significant knowledge gaps in the understanding of graphene growth mechanisms. We enhance current kinetic models through a detailed investigation of C2H2 deposition processes on solid graphene surfaces. These processes represent key elementary reaction steps in the complex heterogeneous network responsible for pyrocarbon formation during chemical vapor deposition and infiltration processes. Unlike previous methodologies that relied on analogies with gas-phase systems, our research meticulously explored the actual system, providing a comprehensive overview of the reactions involved in graphene growth at both armchair and zigzag edges. Utilizing transition state theory, we calculate accurate, temperature-dependent rate constants for all elementary reactions in graphene edge growth. This sheds light on the mechanisms and kinetics of pyrocarbon growth, including the potential for structural defect formation. Findings are compared with analogous gas-phase reactions responsible for soot particle formation, assessing the impact of surface interactions. A lumping technique is applied to reduce the complexity of species and reactions while preserving the accuracy of the chemical description. As such, this approach offers valuable insights into relevant pathways paving the way towards a deep understanding of the chemistry of the pyrolysis of hydrocarbons aiming to produce nanomaterials with targeted properties.
期刊介绍:
Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society.
From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.