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各种化学转化的多功能催化剂的全部潜力仍然没有得到充分开发，主要是因为缺乏对REO系列催化性能的详细基本了解。该项目的目标有两个方面：（i）通过其第一系统量子使整个REO系列的不同催化功能合理化-在原子尺度的化学建模和（ii）使用这些知识，以帮助设计新的催化剂的甲烷氧化偶联（OCM），经济上非常有吸引力，但尚未在实践中实施的天然气转化为增值商品化学品的过程。该项目将寻求一条创新路线，以混合氧化物为基础，进行知识驱动的可调催化剂设计。我们的研究团队旨在为OCM找到高效的催化剂，这是该研究领域取得重大进展的先决条件。REO系列中具有极高的氧迁移率和不同的氧化能力的REO似乎非常适合此目的。REO的计算研究是稀缺的，因为这些系统需要使用先进的电子结构方法和显着的计算能力。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模拟方面的专业知识不断增长，这一复杂的问题终于可以开始了。理论研究将与同一所大学的合作实验组（M. Bäumer）。我们将指导催化剂开发商提出的催化活性的描述符，并通过评估这些描述符在明智地选择的模型系统之前，实际的催化剂制备。

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.