Modeling Activation of Small Molecules by Supported Transition Metals

在化学系化学结构、动力学和机理计划的支持下，明尼苏达大学的克里斯托弗·克雷默教授和他的研究小组将利用量子化学计算方法探索一些重要的化学过程，包括C-H键和分子O2和N2O的活化，以及各种单金属和双金属催化剂体系的水分解。作为对这些特定化学体系的研究的一部分，Cramer团队还将比较密度泛函理论(DFT)计算的结果与实验和/或多参考波函数理论计算的结果。这种比较的目的是验证更简单的密度泛函方法(ES)在涉及前线轨道近简并的复杂问题上的应用。最后，Cramer教授将继续将连续介质溶剂化模型纳入DFT和依赖于时间的DFT(TD-DFT)。除了促进我们对上述特定化学体系的理解外，克雷默教授的研究计划还将促进催化和计算化学领域的发展，并可能对能源转换技术产生影响。该研究计划还将为本科生和研究生的培训提供丰富的环境，克雷默教授和他的团队开展的外联活动将向从高中到高等教育水平的受众介绍计算化学的世界。最后，Cramer教授将在他的下一版教科书“计算化学要点”中包括他的研究结果，并将向其他研究人员提供这项工作产生的任何软件，从而扩大该项目的影响。

In this project supported by the Chemical Structure, Dynamics, and Mechanisms Program of the Division of Chemistry, Professor Christopher Cramer of the University of Minnesota and his research group will employ quantum chemical computational methods to explore a number of important chemical processes, including the activation of C-H bonds and molecular O2 and N2O, and water splitting by various mono-and bimetallic catalyst systems. As part of the investigation into these specific chemical systems, the Cramer team will also compare the results of density functional theory (DFT) calculations with the results of experiment and/or multireference wave function theory calculations. The goal of this comparison is to validate the application of the simpler DFT approach(es) to complex problems involving near degeneracies of frontier orbitals. Finally, Prof. Cramer will continue work on the incorporation of continuum solvation models into DFT and time-dependent DFT (TD-DFT). In addition to advancing our understanding of the specific chemical systems mentioned above, Prof. Cramer's research program will advance the fields of catalysis and computational chemistry, and possibly have implications for energy conversion technology. The research program will also provide a rich environment for the training of undergraduate and graduate students, and outreach activities by Prof. Cramer and his group will introduce the world of computational chemistry to audiences ranging from high school to post-secondary levels. Finally, Prof. Cramer will include results from his research in the next edition of his textbook, "Essentials of Computational Chemistry," and will make any software resulting from this work available to other researchers, thus broadening the impact of the project.