第41卷第2期2024年4月J.At.Mol.Phys.,2024,41:021001(8pp)基于密度泛函理论的CO,吸附微观机理比较研究原子与分子物理学报JOURNALOFATOMICANDMOLECULARPHYSICSVol.41No.2Apr.2024张浩楠，赵兵涛，朱绍良（上海理工大学能源与动力工程学院，上海市200093）摘要：为探究吸附法捕获CO,过程中的微观机理和吸附剂材料间的作用关系，基于密度泛函理论方法，综合比较了典型吸附剂包括煤基官能团、Fe、限域离子液体、Na,CO,、SrTiO,与CO,的吸附过程和差异性：根据不同计算策略，着重分析比较了吸附能、结构优化参数、吸附构型以及原子分布等参数，结果表明，化学吸附中CO,分子与吸附面呈平行关系时通常吸附能最大；在一种材料的同类型官能团中，吸附能大小与氧原子的数量呈正相关关系；吸附过程中C-O键的伸长活化会生成一种重要的中间产物CO，：提出在探寻CO,吸附材料时可以在含氧原子较多的官能团、活性金属表面等方面进一步探究.最后对基于密度泛函理论的CO,的吸附机理的进一步研究方向进行了展望：关键词：密度泛函理论；CO,吸附；吸附能中图分类号：0647.31MicroscopicmechanismofCO,adsorptionbasedondensityfunctionaltheory文献标识码：ADOI;10.19855/j.1000-0364.2024.021001ZHANGHao-Nan,ZHAOBing-Tao,ZHUShao-Liang(CollageofEnergyandPowerEngineering,UniversityofShanghaiforScienceandTechnology,Shanghai200093,China)Abstract:InordertoinvestigatethemicroscopicmechanismandtherelationshipbetweenadsorbentmaterialsintheprocessofCO,capturebyadsorption,theadsorptionprocessesanddifferencesbetweentypicaladsorbentsin-cludingcoal-basedfunctionalgroups,Fe,restrictedionicliquids,Na,CO,andSrTiO,withCO,werecomparedbasedonthedensityfloodingtheoryapproach.Accordingtodifferentcalculationstrategies,theparametersofad-sorptionenergy,structuraloptimizationparameters,adsorptionconfigurationandatomicdistributionareanalyzedandcompared.TheresultsshowthattheadsorptionenergyisusuallyhighestwhentheCO,moleculeisparalleltotheadsorptionsurfaceinchemisorption;theadsorptionenergyispositivelycorrelatedwiththenumberofoxygenatomsinthesametypeoffunctionalgroupofamaterial;andtheelongationactivationoftheC-ObondduringadsorptionproducesanimportantintermediateproductCO,.ItisproposedthatthesearchforCO2...
