摘要
基于密度泛函理论,采用了Dmol3模块对几种不同元素(Fe、Ni、Cu、Zn、Pd和Si)掺杂MoS2所形成的单原子催化剂的性能进行了第一性原理计算。首先分析了掺杂元素与载体之间的结合强度,发现Fe、Ni和Si与MoS2具有良好的结合稳定性。另外,分析了几种X-MoS2对CO催化氧化的性能,计算比较了对CO和O2的吸附能,遵循顺序如下:Pd<Cu<Ni<Fe<Si。其中,Si-MoS2表现出了优异的催化性质,对O2的吸附能最大且明显高于CO。通过E-R机理分析表明,这将有利于O2在催化活性位点被高效活化,保证下一步CO氧化反应的进行。通过局域态密度分析,与CO相比,在费米能级附近Si和O2产生的相互作用明显更强,其对O2的吸附作用也更强。Si掺杂MoS2具有成为CO氧化反应催化剂的潜力。
Based on the density functional theory,the first-principle calculation of the performance of single atom catalysts,MoS2 doped with several different elements(Fe,Ni,Cu,Zn,Pd and Si),was carried out by the Dmol3 module.Firstly,the bonding strength between the doped elements and the support was analyzed.It was found that Fe,Ni and Si have good bonding stability with MoS 2.In addition,the performance of several X-MoS2 catalysts for CO oxidation was analyzed,and the adsorption energy of CO and O2 were calculated and compared.The following order was followed:Pd<Cu<Ni<Fe<Si.Among them,Si-MoS2 shows excellent catalytic properties,and the adsorption energy of O2 was the largest and significantly higher than that of CO.The E-R mechanism analysis shows that it would be conducive to the efficient activation of O2 at the catalytic active site and ensure the next CO oxidation reaction.The analysis of local density of states show that the interaction between Si and O2 near Fermi level is stronger than that of CO,so the adsorption of O2 is stronger than that of CO.Si doped MoS2 has the potential to be a catalyst for CO oxidation.
作者
王克良
李静
黄禹
连明磊
范佳鑫
WANG Keliang;LI Jing;HUANG Yu;LIAN Minglei;FAN Jiaxin(College of Chemistry and Materials Engineering,Liupanshui Normal University,Liupanshui 553004,China;College of Chemistry and Chemical Engineering,Guizhou University,Guiyang 550025,China)
出处
《人工晶体学报》
EI
CAS
北大核心
2020年第4期672-676,共5页
Journal of Synthetic Crystals
基金
贵州省科技厅联合基金(黔科合J字LKLS[2013]27号)
贵州省教育厅青年科技人才项目(黔教合KY字[2019]137)
卓越工程师培养计划(LPSSYzyjypyjh201702)
贵州省教育厅特色重点实验室项目([2011]278)
煤基清洁能源应用与转化科技创新团队(LPSSYKJTD201908)。
