Fe、Ir掺杂MoS_(2)表面对N_(2)气敏吸附与解离反应性能提升的第一性原理研究  

First-principles study on the improvement of N_(2) gas sensitive adsorption and dissociation reaction performance on Fe and Ir doped MoS_(2) surfaces

作　　者：肖香珍[1] 胡林峰[1] 张建伟[1] XIAO Xiang-Zhen;HU Lin-Feng;ZHANG Jian-Wei(Henan Institute of Science and Technology,Xinxiang 453003,China)

机构地区：[1]河南科技学院,新乡453003

出　　处：《原子与分子物理学报》2025年第1期13-19,共7页Journal of Atomic and Molecular Physics

基　　金：河南省科技攻关项目(212102110148)。

摘　　要：基于第一性原理方法,采用周期性平板模型,研究了N_(2)分子在掺杂体系TM-MoS_(2)(TM=Fe、Ir)表面的吸附和解离行为.研究表明:N_(2)分子在TM-MoS_(2)(TM=Fe、Ir)表面吸附能依次为0.62和0.47 eV,而完整MoS_(2)表面的吸附能只有0.08 eV,说明掺杂之后对N_(2)表现出略好的吸附性能.差分电荷密度分析表明,N_(2)吸附后,掺杂Fe、Ir原子与两个N原子之间电荷有所增加,N-N键之间的区域电荷密度减少,N-N键的强度减弱.态密度计算结果发现,N_(2)在吸附过程中,主要是N原子的2p_(y)、2p_(z)轨道与Ir的5d_(xy)和5d_(z^(2))以及Fe的3d_(xy)和3d_(z^(2))发生杂化作用.通过分析解离活化能,N_(2)在掺杂体系TM-MoS_(2)(TM=Fe、Ir)表面解离需要活化能均较高,且远大于在相应掺杂表面的吸附能,说明N_(2)在掺杂体系TM-MoS_(2)(TM=Fe、Ir)表面解离应该表现为分子吸附或脱附.The adsorption and dissociation behaviors of N_(2) molecules on the surfaces of TM-MoS_(2)(TM=Fe,Ir)doped systems were studied by using the first principles methods with the periodic slab model.The study shows that:the adsorption energies of N_(2) molecules on the TM-MoS_(2)(TM=Fe,Ir)surfaces are 0.62 and 0.47 eV in turn,while that on the intact MoS_(2) surface is only 0.08 eV,indicating that doping followed by N_(2) exhibits slightly better adsorption performance.Differential charge density analysis showed that after N_(2) adsorption,the charge between doped Fe or Ir atom and two N atoms is increased,the charge density in the region between the N-N bond is decreased,and the strength of the N-N bond is weakened.The density of states calculations revealed that N_(2) mainly undergoes hybridization between the 2p_(y) and 2p_(z) orbitals of N atoms and the 5d_(xy) and 5d_(z^(2)) of Ir,as well as the 3d_(xy) and 3d_(z^(2))of Fe during the adsorption process.By analyzing the dissociation activation energy,the dissociation of N_(2) on the surface of TM-MoS_(2)(TM=Fe,Ir)in the doped system requires that the activation energy is both higher and much larger than that on the corresponding doped surface,which indicates that N_(2) dissociation on the surface of TM-MoS_(2)(TM=Fe,Ir)in the doped system should show molecular adsorption or desorption.

关 键 词：Fe、Ir 掺杂 单层MoS_(2) N_(2) 吸附与解离 活化能 密度泛函理论 

分 类 号：O641[理学—物理化学]