Combinatorial Screening of Supports and Additives by Means of Accelerated Quantum Chemical Molecular Dynamics Method

环境催化剂在解决环境问题中发挥着重要作用。这些都有望成为实现绿色化学过程的关键技术。我们最近将组合方法引入到催化剂设计的计算化学中，并提出了一种称为“组合计算化学”的新方法。此外，我们还成功地开发了一种新的大规模模型加速量子化学分子动力学程序，称为“颜色”。这个程序比常规的第一性原理方法快5000倍。在上述方法的基础上，我们尝试实现由催化种类、载体材料、助剂组成的催化剂材料的快速筛选。我们的最终目标是设计出具有更高催化性能的环保催化剂。我们成功地从理论上阐明了添加剂对Cu/ZnO甲醇合成催化剂催化活性的影响。实验报道了CO对燃料电池中…More ed Pt电极催化剂的毒性。我们预测Mo添加剂具有较高的抑制Pt电极中毒的能力。在铁基费托催化剂中，Mo是理论上最合适的添加剂。我们还利用复杂的大尺度模型，对铁催化剂上碳化物的形成和氢的反应动力学进行了理性化。另一方面，我们的“Colors”程序的准确性得到了证明，因为“Colors”程序得到的各种催化剂载体（包括稀土氧化物和沸石材料）的电子和原子结构与实验和第一性原理方法得到的结果基本一致。为了揭示载体对催化剂种类的影响，模拟并分析了负载型催化剂大尺度模型的电子结构变化。综上所述，通过“组合计算化学”和“颜色”程序，考虑了由催化物种、支撑材料和添加剂组成的现实复杂大尺度模型，成功地进行了催化剂材料的快速筛选。少

Environmental catalysts play important roles in the solving of environmental problems. These are expected as the key technology which would realize green chemistry processes. We recently introduced the combinatorial approach to computational chemistry for catalyst design and proposed a new method called "Combinatorial Computational Chemistry". Further, we also succeeded to develop a new accelerated quantum chemical molecular dynamics program for large-scale models, called "Colors". This program is 5000 times faster than the regular first-principles approach.Based on the above methods, we attempted to realize the rapid screening of catalysts materials which consist of catalytic species, support materials, and additives. Our final goal is to design environmental catalysts which possess higher catalytic performance. We succeeded to elucidate the effect of additives on the catalytic activity of Cu/ZnO methanol synthesis catalyst theoretically. Experimentally, it was reported that CO poison … More ed Pt electrode catalysts in fuel cells. We predicted that Mo additive possessed the higher ability to suppress the poisoning of Pt electrode. In Fischer-Tropsch catalysts based on Fe, Mo was found to be the most suitable additive theoretically. We also rationalized the dynamics of the formation of carbides and the reaction with hydrogen on the Fe catalysts, by using the complicated large-scale models. On the other hand, the accuracy of our "Colors" program was demonstrated because the electronic and atomic structures of various kinds of catalyst support including rare-earth oxides as well as zeolitic material obtained by "Colors" substantially agreed with those obtained by experiments and first-principles approach. To reveal the effects of support on catatytic species, the variation of the electronic structures of the large-scale models for supported catalysts was simulated and successfully analyzed. As a conclusion, the rapid screening of catalysts materials was successful with considering the realistic complicated large-scale models which consist of catalytic species, support materials, and additives, by means of "Combinatorial Computational Chemistry" and "Colors" program. Less