Development of First-Principle Combinatorial Computational Chemistry Method and Its Application to Catalyst Design

组合化学已经发展成为一种实验方法，可以一次合成数百个样品并检查它们的性质。组合化学最初是在有机化合物的合成中提出并发展起来的。现在，它在药物和生物技术的发展中不可或缺。近年来，组合化学被引入无机化学领域。特别是随着薄膜、发光体、磁电阻等元素体系应用的日益广泛，组合化学有望成为无机材料合成中的高效筛选方法;计算化学则主要用于催化机理、催化活性和失活机理的研究。除了在原子和电子水平上研究众所周知的催化反应的机理外，计算化学也是一门新兴的学科。 ...更多信息 在预测具有高活性、高选择性和高抗毒性的新型催化剂方面具有重要作用。最近，我们将组合方法引入到催化剂设计的计算化学中，提出了一种新的方法，称为“组合计算化学”。该方法利用计算机模拟技术系统地计算了大量金属、载体和添加剂对催化活性的影响，以预测每个催化反应的最佳元素。在本项目中，我们开发了大量第一原理计算化学程序，如（1）加速量子化学分子动力学，（2）开壳层加速量子化学分子动力学，（3）混合第一原理量子化学分子动力学，（4）粗晶晶体生长模拟器，（5）表面化学反应晶体生长模拟器等。此外，我们应用我们的组合计算化学方法设计（1）deNOx催化剂，（2）甲醇合成催化剂，（3）费托合成催化剂等，有力地证实了我们的组合计算化学方法的有效性和适用性。少

Combinatorial chemistry has been developed as an experimental method where it is possible to synthesize hundreds of samples all at once and examine their properties. Originally combinatorial chemistry was proposed and has been developed mainly in the synthesis of organic compounds. Now it is indispensable in the development of drugs and biotechnology. Recently, combinatorial chemistry was introduced into the inorganic field. Especially, because of the increased utility of many elements system, such as thin films, luminous bodies, and magnetoresistances, combinatorial chemistry is expected to work as a highly efficient screening method even in inorganic material synthesis.On the other hand, computational chemistry is used mainly to elucidate the catalytic mechanism, catalytic activity, and deactivation mechanism in the catalysis field. In addition to the investigation of the mechanism of the well known catalytic reactions at atomic and electronic levels, computational chemistry is expec … More ted to have an important role in predicting new catalysts with high activity, high selectivity, and high resistance to poisons. Recently, we introduced the combinatorial approach to computational chemistry for catalyst design and proposed a new method called "combinatorial computational chemistry". In this approach, the effects of a large number of metals, supports, and additives on the catalytic activity are calculated systematically using computer simulation techniques, in order to predict the best element for each catalytic reaction.In this project, we developed a lot of programs for first-principle combinatorial computational chemistry, such as (1) accelerated quantum chemical molecular dynamics, (2) open-shell accelerated quantum chemical molecular dynamics, (3) hybrid first-principle quantum chemical molecular dynamics, (4) coarse-grained crystal growth simulator, (5) crystal growth simulator for surface chemical reactions and so on. Moreover, we applied our combinatorial computational chemistry approach to design (1) deNOx catalysts, (2) methanol synthesis catalysts, (3) Fischer-Tropsh synthesis catalysts, etc. and the effectivity and applicability of our combinatorial computational chemistry approach were strongly confirmed. Less