The development of new density functional based methods and their application to catalysis

点击翻译按钮获取中文摘要

Catalysis is the gentle art of triggering desirable chemical reactions without forceful means such as high pressures or excessive heat. Its practical use has changed the world around us by facilitating the production of an ever-increasing variety of synthetic materials. Other catalysts are employed by nature to convert nitrogen, oxygen and carbon dioxide from the atmosphere into chemicals vital to the ecosystem of our planet. The way in which reactions are triggered by catalysts is often not known in details. Because catalytic processes are fast, they are difficult to follow even by sophisticated experimental detection methods. Fortunately, the rapid developments in computer technology combined with significant advances in modeling methodologies have opened up ways in which catalytic processes can be analyzed by computer simulation. It is the objective of the proposed research to explore these possibilities further. We have adopted Density Functional Theory (DFT) as our theoretical model. A considerable program system called ADF (Amsterdam Density Functional program) has been developed over the past 30 years for calculations on digital computers in collaboration with the theory group of Professor E.J. Baerends at the Free University in Amsterdam. It is the long term goal to develop ADF into a multi-scale simulation package for use in chemistry, solid state physics, biology and surface science. ADF has currently some 1000 users in industry, government, and academia. Our own developments over the next 5 years will entail methodologies that can make the study of chemical reactions involving transition metal centers more tractable. In contrast to previous years, more emphasis will be given to reactions on the potential energy surface of periodic systems.We are further involved with the development and implementation of a new theory that should make it possible to calculate excited state properties with high accuracy using DFT-based methods.