{"title":"PEI捕集CO2: LPEI和BPEI最终氧化稳定性的分子模拟研究","authors":"Wim Buijs*, ","doi":"10.1021/acsengineeringau.2c00033","DOIUrl":null,"url":null,"abstract":"<p >Amine resins are frequently studied to capture CO<sub>2</sub> from industrial emission sources and air. Polyethylene imine (PEI) is a typical example showing relatively high CO<sub>2</sub> uptake and not too energy demanding desorption of CO<sub>2</sub>. For practical application, its oxidation stability is of great importance. In this DFT study, the ultimate oxidation stability of the two forms of PEI, linear PEI (LPEI) and branched PEI (BPEI), is investigated. First, the oxidation stability order for amines was determined using small amine clusters: primary > secondary > tertiary amines. Using LPEI and BPEI structure-related clusters, it turned out that under optimal conditions, the formation of α-amino hydroperoxide of PEI is the rate-determining step. Optimal conditions are the total absence of initiators like transition-metal ions, NO<sub><i>x</i></sub>, O<sub>3</sub>, or hydrocarbons and the presence of H<sub>2</sub>O and CO<sub>2</sub>. All computational results are in line with experimental results.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":4.3000,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.2c00033","citationCount":"1","resultStr":"{\"title\":\"CO2 Capture with PEI: A Molecular Modeling Study of the Ultimate Oxidation Stability of LPEI and BPEI\",\"authors\":\"Wim Buijs*, \",\"doi\":\"10.1021/acsengineeringau.2c00033\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Amine resins are frequently studied to capture CO<sub>2</sub> from industrial emission sources and air. Polyethylene imine (PEI) is a typical example showing relatively high CO<sub>2</sub> uptake and not too energy demanding desorption of CO<sub>2</sub>. For practical application, its oxidation stability is of great importance. In this DFT study, the ultimate oxidation stability of the two forms of PEI, linear PEI (LPEI) and branched PEI (BPEI), is investigated. First, the oxidation stability order for amines was determined using small amine clusters: primary > secondary > tertiary amines. Using LPEI and BPEI structure-related clusters, it turned out that under optimal conditions, the formation of α-amino hydroperoxide of PEI is the rate-determining step. Optimal conditions are the total absence of initiators like transition-metal ions, NO<sub><i>x</i></sub>, O<sub>3</sub>, or hydrocarbons and the presence of H<sub>2</sub>O and CO<sub>2</sub>. All computational results are in line with experimental results.</p>\",\"PeriodicalId\":29804,\"journal\":{\"name\":\"ACS Engineering Au\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.3000,\"publicationDate\":\"2022-12-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.2c00033\",\"citationCount\":\"1\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Engineering Au\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsengineeringau.2c00033\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Engineering Au","FirstCategoryId":"1085","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsengineeringau.2c00033","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
CO2 Capture with PEI: A Molecular Modeling Study of the Ultimate Oxidation Stability of LPEI and BPEI
Amine resins are frequently studied to capture CO2 from industrial emission sources and air. Polyethylene imine (PEI) is a typical example showing relatively high CO2 uptake and not too energy demanding desorption of CO2. For practical application, its oxidation stability is of great importance. In this DFT study, the ultimate oxidation stability of the two forms of PEI, linear PEI (LPEI) and branched PEI (BPEI), is investigated. First, the oxidation stability order for amines was determined using small amine clusters: primary > secondary > tertiary amines. Using LPEI and BPEI structure-related clusters, it turned out that under optimal conditions, the formation of α-amino hydroperoxide of PEI is the rate-determining step. Optimal conditions are the total absence of initiators like transition-metal ions, NOx, O3, or hydrocarbons and the presence of H2O and CO2. All computational results are in line with experimental results.
期刊介绍：
）ACS Engineering Au is an open access journal that reports significant advances in chemical engineering applied chemistry and energy covering fundamentals processes and products. The journal's broad scope includes experimental theoretical mathematical computational chemical and physical research from academic and industrial settings. Short letters comprehensive articles reviews and perspectives are welcome on topics that include:Fundamental research in such areas as thermodynamics transport phenomena (flow mixing mass & heat transfer) chemical reaction kinetics and engineering catalysis separations interfacial phenomena and materialsProcess design development and intensification (e.g. process technologies for chemicals and materials synthesis and design methods process intensification multiphase reactors scale-up systems analysis process control data correlation schemes modeling machine learning Artificial Intelligence)Product research and development involving chemical and engineering aspects (e.g. catalysts plastics elastomers fibers adhesives coatings paper membranes lubricants ceramics aerosols fluidic devices intensified process equipment)Energy and fuels (e.g. pre-treatment processing and utilization of renewable energy resources; processing and utilization of fuels; properties and structure or molecular composition of both raw fuels and refined products; fuel cells hydrogen batteries; photochemical fuel and energy production; decarbonization; electrification; microwave; cavitation)Measurement techniques computational models and data on thermo-physical thermodynamic and transport properties of materials and phase equilibrium behaviorNew methods models and tools (e.g. real-time data analytics multi-scale models physics informed machine learning models machine learning enhanced physics-based models soft sensors high-performance computing)
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