General Structure-Reactivity Relationship for Oxygen on Transition-Metal Oxides
General Structure-Reactivity Relationship for Oxygen on Transition-Metal Oxides
复制标题
氧在过渡金属氧化物上的一般结构-反应关系
DOI：
10.1021/acs.jpclett.7b00861
复制
发表时间：
2017-05-18
影响因子：
5.7
通讯作者：
Jiang, De-en
中科院分区：
文献类型：
--
作者：
Fung, Victor;Tao, Franklin Feng;Jiang, De-en
尽管最近在设计和筛选催化剂以提高性能方面取得了许多进展，但过渡金属氧化物仍然被证明是具有挑战性的，因为系统的内在复杂性和它们可能表现出的可能的形态。在此，我们提出了一个结构描述符，即调整配位数（ACN），它可以概括过渡金属氧化物许多可能的表面表面和缺陷上氧位的反应性。我们证明了这种几何描述符与四种过渡金属氧化物在五个方面的活性位点的电子和能量特性之间的强相关性。然后，我们使用结构描述符来预测C-H活化能，以显示使用ACN预测催化性能的巨大潜力。本研究首次探讨了过渡金属氧化物催化剂活性位点结构与反应活性之间的定量关系。
Despite many recent developments in designing and screening catalysts for improved, performance, transition-metal oxides continue to prove to be challenging due to the myriad inherent complexities of the systems and the possible morphologies that they can exhibit. Herein we propose a structural descriptor, the adjusted coordination number (ACN), which can generalize the reactivity of the oxygen sites over the many possible surface facets and defects of a transition-metal oxide. We demonstrate the strong correlation of this geometric descriptor with the electronic and energetic properties of the active sites on five facets of four transition-metal oxides. We then use the structural descriptor to predict C-H activation energies to show the great potential of using ACN for the prediction of catalytic performance. This study presents a first look into quantifying the relation between active site structure and reactivity of transition metal-oxide catalysts.