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

稀土氧化物(REO)作为具有巨大经济前景的多种化学转化催化剂的全部潜力仍未得到充分开发，这主要是因为对REO系列的催化性质缺乏详细的基础了解。该项目的目标有两个：(I)通过首次在原子尺度上进行系统的量子化学模拟，使整个REO系列的不同催化功能合理化；(Ii)利用这些知识帮助设计新的甲烷氧化偶联催化剂(OCM)，这是一种在经济上非常有吸引力的过程，但尚未在实践中实施，将天然气转化为增值的商品化学品。该项目将探索一条知识驱动的基于混合氧化物的可调催化剂设计的创新路线。我们的研究团队致力于为OCM找到一种高效的催化剂，这是该研究领域取得重大进展的先决条件。REO系列中的REO具有极高的氧迁移率和不同的氧化能力，似乎非常适合这一目的。对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，随着计算化学的不断进步，新的计算工具的出现，以及计算界在多相催化反应理论建模方面的专业知识不断增长，这一复杂的问题终于准备好开始了。理论研究将与同一所大学的合作实验小组(M.Bäumer教授)的活动并行进行。我们将通过建议催化剂活性的描述符并在实际制备催化剂之前在明智地选择的模型系统中评估这些描述符来指导催化剂开发者。

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.