戚春保,王涛,王金涛,陶思昊,秦铭澳.CO2 δ-Pu(100)表面吸附行为的第一性原理研究[J].稀有金属材料与工程,2021,50(8):2728~2737.[Qi Chunbao,Wang Tao,Wang Jintao,Tao Sihao,Qin Ming'ao.Study on Adsorption Behavior of CO2 on the δ-Pu(100) Sur-face Based on First-principles[J].Rare Metal Materials and Engineering,2021,50(8):2728~2737.]
CO2 δ-Pu(100)表面吸附行为的第一性原理研究
投稿时间:2020-07-04  修订日期:2020-08-25
中文关键词:  钚表面  CO2  密度泛函  电子密度  吸附行为  作用机理
基金项目:
中文摘要:
      结合密度泛函理论框架内的周期性平板模型,运用第一性原理计算方法研究了CO2δ-Pu(100)表面的吸附行为。结果表明,CO2分子以C端向下和C-Pu、O-Pu多键结合的方式吸附在δ-Pu(100)表面。吸附类型属于强化学吸附,最稳定的吸附构型是H1-C4O4,此时吸附能为-6.430 eV,吸附稳定性顺序为穴位>桥位>顶位。CO2分子主要和表面Pu原子反应,而与其它3层Pu原子的反应较弱。更多的电子向CO2 u轨道转移有利于C-O键的弯曲和活化。此外,CO2分子和Pu原子之间的化学键主要是离子态,反应机理是CO2的C 2s、C 2p、O 2s 和O 2p轨道与Pu 6p、Pu 6d、Pu 5f轨道发生了重叠杂化作用,产生了新的键结构。H1-C4O4构型的功函数变化最小,表明其它电子容易从该构型表面逃逸,且需要的能量最小。
Study on Adsorption Behavior of CO2 on the δ-Pu(100) Sur-face Based on First-principles
英文关键词:plutonium surface  carbon dioxide  density functional theory  electron density  adsorption behavior  reaction mechanism
英文摘要:
      A first-principles calculation was applied to study the adsorption behavior of CO2 on δ-Pu(100) surface using a slab model within the framework of density functional theory. Results demonstrate that CO2 molecules are adsorbed on δ-Pu(100) surface at C-terminated bent state by multi-bond binding of C-Pu and O-Pu. The adsorption type belongs to strong chemical adsorption and the most stable adsorption configuration is H1-C4O4 with the adsorption energy of -6.430 eV. The adsorption stability order is hollow site>bridge site>top site. CO2 molecule mainly interacts with Pu surface atoms, while the interaction with other three Pu atoms is weak. The transfer of more electrons to the CO2 u orbital is beneficial to the bending and activation of C-O bonds. Moreover, the chemical bonding between Pu atoms and CO2 molecule is mainly ionic state and the reaction mechanism is that the C 2s, C 2p, O 2s and O 2p orbitals of CO2 molecule hybrid with Pu 6p, Pu 6d and Pu 5f orbitals, resulting in a new bond structure. The work function of the H1-C4O4 site changes the least, indicating that other electrons readily escape from the metal surface and the required energy is the smallest.
作者单位E-mail
戚春保 火箭军工程大学 研究生院陕西 西安 710025 za7966093@qq.com 
王涛 火箭军工程大学 核工程学院陕西 西安 710025  
王金涛 火箭军工程大学 核工程学院陕西 西安 710025 wangjintaolove@126.com 
陶思昊 火箭军工程大学 研究生院陕西 西安 710025 1114313684@qq.com 
秦铭澳 火箭军工程大学 研究生院陕西 西安 710025 92420726@qq.com 
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