Theoretical investigation of carbon dioxide adsorption on MgH_(2) with a cobalt catalyst  

作　　者：Sara Rozas Fabiana C.Gennari Mert Atilhan Alfredo Bol Santiago Aparicio 

机构地区：[1]Department of Chemistry,University of Burgos,09001 Burgos,Spain [2]National Scientific and Technical Research Council(CONICET),Bariloche Atomic Centre(CNEA),R8402AGP,S.C.de Bariloche,Rio Negro,Argentina [3]Department of Chemical and Paper Engineering,Western Michigan University,Kalamazoo,MI 49008-5462,USA [4]Department of Physics,University of Burgos,09001 Burgos,Spain [5]International Research Center in Critical Raw Materials for Advanced Industrial Technologies(ICCRAM),University of Burgos,09001 Burgos,Spain

出　　处：《Industrial Chemistry & Materials》2024年第4期587-599,共13页工业化学与材料（英文）

基　　金：This investigation was funded by the CO_(2)absorbing Materials Project-RISE(CO2MPRISE)which received funding from the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant Agreement No.H2020-MSCA-RISE-2016-CO2MPRISE-734873。

摘　　要：This work presents a theoretical investigation of carbon dioxide(CO_(2))adsorption on MgH_(2) and its reaction(chemisorption)with cobalt doped MgH_(2).The focus of this study is the properties and mechanisms involved in CO_(2) adsorption on clean MgH_(2) surfaces and the role of Co in enhancing the adsorption process.Density functional theory(DFT)calculations were performed to examine different CO_(2) adsorption sites on the MgH_(2) surface along with the adsorption distances,binding energies,and geometric parameters.The results indicate that physical adsorption of CO_(2) occurs on MgH_(2) with similar adsorption energies at different adsorption sites.The coverage effect of CO_(2) molecules on MgH_(2) was also investigated,revealing an increased affinity of CO_(2) with higher surface coverage.However,excessive coverage led to a decrease in adsorption efficiency due to competing surface adsorption and intermolecular interactions.The orientation of adsorbed CO_(2) molecules shifted from parallel to quasiperpendicular arrangements upon adsorption,with notable deformations observed at higher coverage,which gives a hint of CO_(2) activation.Furthermore,the study explores the CO_(2) adsorption capacity of MgH_(2) in comparison to other materials reported in the literature,showcasing its medium to strong affinity for CO_(2).Additionally,the effectiveness of a single Co atom and Co clusters as catalysts for CO_(2) adsorption on MgH_(2) was examined.Overall,this theoretical investigation provides insights into the CO_(2) adsorption properties of MgH_(2) and highlights the potential of Co catalysts to enhance the efficiency of the methanation process.

关 键 词：DFT CO_(2)conversion Cobalt catalyst Charge transfer 

分 类 号：O64[理学—物理化学]