Reuter Karsten, Plaisance Craig P, Oberhofer Harald, Andersen Mie
Chair for Theoretical Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstr. 4, D-85747 Garching, Germany.
J Chem Phys. 2017 Jan 28;146(4):040901. doi: 10.1063/1.4974931.
First-principles screening approaches exploiting energy trends in surface adsorption represent an unparalleled success story in recent computational catalysis research. Here we argue that our still limited understanding of the structure of active sites is one of the major bottlenecks towards an ever extended and reliable use of such computational screening for catalyst discovery. For low-index transition metal surfaces, the prevalently chosen high-symmetry (terrace and step) sites offered by the nominal bulk-truncated crystal lattice might be justified. For more complex surfaces and composite catalyst materials, computational screening studies will need to actively embrace a considerable uncertainty with respect to what truly are the active sites. By systematically exploring the space of possible active site motifs, such studies might eventually contribute towards a targeted design of optimized sites in future catalysts.
利用表面吸附中的能量趋势的第一性原理筛选方法是近期计算催化研究中一个无与伦比的成功案例。在此我们认为，我们对活性位点结构的理解仍然有限，这是在催化剂发现中更广泛、可靠地使用此类计算筛选的主要瓶颈之一。对于低指数过渡金属表面，由名义上的体截断晶格提供的普遍选择的高对称（平台和台阶）位点可能是合理的。对于更复杂的表面和复合催化剂材料，计算筛选研究将需要积极面对关于真正的活性位点是什么存在的相当大的不确定性。通过系统地探索可能的活性位点基序空间，此类研究最终可能有助于未来催化剂中优化位点的靶向设计。
