Npj Comput. Mater.: 单原子催化剂动态电荷转移—找CeO2试一下
海归学者发起的公益学术平台
分享信息，整合资源
交流学术，偶尔风月
单原子催化剂是一种有前景的材料，它可以充分地利用活性位点，提高催化效率。迄今，各类衬底材料都已经被用于制备单原子催化剂，如其他金属、掺杂的碳、金属有机框架和最常见的氧化物材料，等等。氧化物上单原子的稳定性通常归因于其较强的金属-载体相互作用，其电子可以从金属转移给载体，也可以从载体转移给金属，因而导致金属原子电子结构性质的改变。例如，由于金属和二氧化铈衬底的电子耦合作用，Pt1/CeO2体系中孤立Pt原子的氧化态会发生动态变化。这种动态效应显著增加了结构和电子的复杂性，使预测动态行为具有挑战性。
该文近期发表于npj Computational Materials 8：171(2022)，英文标题与摘要如下，点击左下角“阅读原文”可以自由获取论文PDF。
Data-driven models for ground and excited states for Single Atoms on Ceria
Julian Geiger, Albert Sabadell-Rendón, Nathan Daelman & Núria López
Ceria-based single-atom catalysts present complex electronic structures due to the dynamic electron transfer between the metal atoms and the semiconductor oxide support. Understanding these materials implies retrieving all states in these electronic ensembles, which can be limiting if done via density functional theory. Here, we propose a data-driven approach to obtain a parsimonious model identifying the appearance of dynamic charge transfer for the single atoms (SAs). We first constructed a database of (701) electronic configurations for the group 9–11 metals on CeO2(100). Feature Selection based on predictive Elastic Net and Random Forest models highlights eight fundamental variables: atomic number, ionization potential, size, and metal coordination, metal–oxygen bond strengths, surface strain, and Coulomb interactions. With these variables a Bayesian algorithm yields an expression for the adsorption energies of SAs in ground and low-lying excited states. Our work paves the way towards understanding electronic structure complexity in metal/oxide interfaces.
扩展阅读
微信扫码关注该文公众号作者