Tang Hairong, Trout Bernhardt L
Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA.
J Phys Chem B. 2005 Apr 21;109(15):6948-51. doi: 10.1021/jp050483z.
We have developed a new electronic composition-property relationship between the adsorption energy of molecules binding unequally to multiple atoms on metal surfaces and the electronic properties of the surface. This relationship allows the estimation of the relative stability of adsorbates on various surfaces, assuming that the adsorbate adopts the same local configuration on each surface, and therefore also allows the estimation of the adsorption energy of molecules through large regions of parameter space in alloy systems with data from only a few explicit calculations. We have applied this relationship to the adsorption of SO(2) on Pt surfaces alloyed with Pd, Cu, Ru, and Ni. Using a new formula for weighting the metal d-band, we found a strong linear relationship between the weighted positions of the d states of surfaces and the most stable molecular adsorption energies. The consequences of our electronic composition-property relationship for catalyst design are also discussed.
我们已经建立了一种新的电子组成-性质关系，该关系存在于分子在金属表面与多个原子不等同结合的吸附能和表面的电子性质之间。这种关系允许估计吸附质在各种表面上的相对稳定性，前提是吸附质在每个表面上采用相同的局部构型，因此也允许通过合金系统中仅来自少数显式计算的数据来估计分子在大参数空间区域内的吸附能。我们已将这种关系应用于SO(2)在与Pd、Cu、Ru和Ni合金化的Pt表面上的吸附。使用一种加权金属d带的新公式，我们发现表面d态的加权位置与最稳定的分子吸附能之间存在很强的线性关系。我们还讨论了这种电子组成-性质关系对催化剂设计的影响。
