Ko Jeonghyun, Kwon Hyunguk, Kang Hyejin, Kim Byung-Kook, Han Jeong Woo
Department of Chemical Engineering, University of Seoul, Seoul 130-743, Korea.
Phys Chem Chem Phys. 2015 Feb 7;17(5):3123-30. doi: 10.1039/c4cp04770b. Epub 2014 Dec 17.
Understanding the adsorption phenomena of small adsorbates involved in surface reactions on transition metals is important because their adsorption strength can be a descriptor for predicting the catalytic activity. To explore adsorption energies on a wide range of binary transition metal alloys, however, tremendous computational efforts are required. Using density functional theory (DFT) calculations, here we suggest a "surface mixing rule" to predict the adsorption energies of H, O, S, CO and OH on bimetallic alloys, based on the linear interpolation of adsorption energies on each pure surface. As an application, the activity of CO oxidation on various bimetallic alloys is predicted from the adsorption energies of CO and O easily obtained by the surface mixing rule. Our results provide a useful tool for rapidly estimating adsorption energies, and furthermore, catalytic activities on multi-component metal alloy surfaces.
理解参与过渡金属表面反应的小分子吸附质的吸附现象非常重要，因为它们的吸附强度可以作为预测催化活性的一个描述符。然而，要探索各种二元过渡金属合金上的吸附能，需要巨大的计算量。在这里，我们利用密度泛函理论（DFT）计算，基于各纯表面吸附能的线性插值，提出了一个“表面混合规则”来预测H、O、S、CO和OH在双金属合金上的吸附能。作为一个应用，通过表面混合规则容易获得的CO和O的吸附能来预测各种双金属合金上CO氧化的活性。我们的结果为快速估计吸附能以及多组分金属合金表面的催化活性提供了一个有用的工具。
