Understanding the catalytic performance of rare-earth oxides: Toward a knowledge-driven design of catalysts from first-principles calculations

稀土氧化物（REOs）作为各种化学转化的多功能催化剂的全部潜力和巨大的经济前景仍未得到充分的探索，主要是因为缺乏对REO系列催化性能的详细基本了解。该项目的目标是双重的：(i)通过他们在原子尺度上的第一个系统量子化学模型来使整个REO系列的不同催化功能变得合理；（ii）利用这些知识来帮助设计用于甲烷氧化偶联的新催化剂（OCM），这是一种经济上极具吸引力的催化剂，但尚未在将天然气转化为增值商品化学品的实践过程中实施。该项目将在混合氧化物的基础上寻求知识驱动的可调催化剂设计的创新路线。我们的研究团队旨在寻找一种高效的OCM催化剂，这是该研究领域取得重大进展的先决条件。REO系列中具有极高氧迁移率和不同氧化能力的REO似乎非常适合这一目的。reo的计算研究很少，因为这些系统需要使用先进的电子结构方法和强大的计算能力。如今，随着计算化学的进步，新的计算工具的可用性，以及计算界在多相催化反应理论建模方面的专业知识的增长，这个复杂的问题终于准备好着手研究了。理论研究将与同一所大学的合作实验小组（M.教授Bäumer）的活动同时进行。我们将通过提出催化活性的描述符并在实际催化剂制备之前在明智选择的模型系统中评估这些描述符来指导催化剂开发人员。

The full potential of rare earth oxides (REOs) as versatile catalysts for various chemical transformations with great economic promise is still quite underexplored mainly because a detailed fundamental understanding of the catalytic properties of the REO series is lacking.The goal of the project is two-fold: (i) rationalize different catalytic function of the whole REO series through their first systematic quantum-chemical modelling at an atomic scale and (ii) use this knowledge to help design new catalysts for the oxidative coupling of methane (OCM), an economically highly attractive but not yet implemented in practice process for conversion of natural gas into value-added commodity chemicals. The project will pursue an innovative route for knowledge-driven design of tunable catalysts on the basis of mixed oxides. Our research team aims at finding a highly efficient catalyst for OCM, which is a prerequisite for a major advancement in this field of research. REOs with their exceptionally high oxygen mobility and varying oxidizing capability within the REO series seem to be ideally suitable for this purpose. Computational studies of REOs are scarce because these systems require the use of advanced electronic-structure methods and significant computing power. Nowadays, with increased progress in computational chemistry, the availability of new computational tools, and with the growing expertise of the computational community in theoretical modelling of heterogeneous catalytic reactions, this complex matter is finally ready to be embarked on. The theoretical study will be carried out in parallel with the activities of the collaborating experimental group at the same university (Prof. M. Bäumer). We will guide catalyst developers by suggesting descriptors of the catalytic activity and by evaluating these descriptors in judiciously selected model systems before actual catalysts are prepared.