论文标题
通过非弹性中子散射和密度功能理论计算，探测霍夫曼外lates中的SO $ _2 $吸附机制
Probing the SO$_2$ adsorption mechanism in Hofmann clathrates via inelastic neutron scattering and density functional theory calculations
论文作者
论文摘要
使用非弹性中子中子散射和密度功能理论计算，研究了Hofmann样配位聚合物Fe（PZ）[PT（CN）4]中SO2的吸附机制。我们发现气体吸附时最重要的光谱变化是在100 cm-1处发现的低能峰的蓝光，这一特征已通过计算出的中子加权状态的声子密度完全证实。我们的计算表明，这种变化的起源是双重的：i）由于气体与PT（CN）4平面的结合而导致氰化物平面运动的力常数增加，而II）由于空间阻碍而导致吡嗪的阻碍旋转。中子散射数据的高能量区域的光谱重量由吡嗪的内部振动所支配的，这可能会受到气体的存在的影响，这正如结合的物理吸附类型所预期的那样。
The adsorption mechanism of SO2 in the Hofmann-like coordination polymer Fe(pz)[Pt(CN)4] is studied using inelastic neutron scattering and density functional theory calculations. We find that the most important spectral change upon gas adsorption is the blueshift of the low energy peak found at 100 cm-1, a feature that is fully confirmed by the computed neutron-weighted phonon density of states. Our calculations suggest that the origin of this change is twofold: i) an increase in the force constant of the cyanide out-of-plane movement due to the binding of the gas onto the Pt(CN)4 plane, and ii) the hampered rotation of the pyrazine due to steric hindrance. The high energy region of the neutron scattering data whose spectral weight is dominated by the internal vibrations of the pyrazine is negligibly affected by the presence of the gas as expected from a physisorption type of binding.
