O2在δ-Pu(100)表面吸附行为的第一原理研究

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采用密度泛函理论结合周期性平板模型研究了O_2分子在δ-Pu(100)表面的吸附行为。结果表明O_2在δ-Pu表面吸附时分子键长增加并最终断裂,离解成2个原子态吸附,离解后的氧原子以心位和桥位吸附优先。最可能的吸附过程为:桥位平行吸附后2个氧原子处于2个心位;心位平行吸附的O_2分子通过旋转平移后,离解为一个心位和一个桥位吸附的氧原子。吸附能大小为2个氧原子的吸附能减去氧分子离解能。自旋限制和自旋极化2种水平计算获得的最稳定吸附方式吸附能分别为8.14 eV和7.29 eV。离解吸附后的电荷布局数,诱导表面功函、电子态等和单个O原子吸附结果一致。 Adsorption behavior of O_2 on δ-Pu (100) surface has been studied by using density functional theory and periodic flat model. The results showed that the molecular bond of O_2 increased and finally ruptured when it adsorbed on δ-Pu surface, which was dissociated into two atomic states. The dissociated oxygen atoms were preferentially adsorbed at the core and bridge sites. The most likely adsorption process is that the two oxygen atoms are located at two positions after parallel adsorption of bridge sites. O_2 molecules adsorbed parallel to each other in the position of the center of gravity are separated into a single position and one oxygen atom adsorbed at the bridge position by rotational translation. The adsorption energy of two oxygen atoms minus the molecular dissociation energy of oxygen. The most stable adsorption mode adsorption energies calculated by spin-spin and spin-polarization calculations are 8.14 eV and 7.29 eV, respectively. The number of charges after dissociative adsorption, induced surface work function, electronic state and the same single O atom adsorption results.
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