近日，英国剑桥大学Michaelides, Angelos团队提出了离子材料表面化学建模的一个准确和有效的框架。相关论文于2025年8月13日发表在《自然-化学》杂志上。

量子力学模拟可以提供对表面化学过程的原子水平的见解，这对于推进异质催化、能量储存和温室气体封存的应用至关重要。不幸的是，事实证明，实现可靠预测所需的准确性具有挑战性。密度泛函理论因其效率而受到广泛关注，但它可能不一致，因此需要相关波函数理论的精确方法。但是高计算需求和大量的主题干预传统上使得相关波函数理论在表面上不可行。

研究组提出了一个自动化框架，利用多层嵌入方法将相关波函数理论应用于离子材料的表面，其计算成本接近密度泛函理论。有了这个框架，他们重现了19种不同吸附表面系统的实验吸附焓。研究组进一步解决了关于几种系统的吸附配置的争论，同时提供了评估密度泛函理论的基准。这个框架是开放的，有利于相关波函数理论在涉及离子材料表面的复杂问题中的常规应用。

附：英文原文

Title: An accurate and efficient framework for modelling the surface chemistry of ionic materials

Author: Shi, Benjamin X., Rosen, Andrew S., Schfer, Tobias, Grneis, Andreas, Kapil, Venkat, Zen, Andrea, Michaelides, Angelos

Issue&Volume: 2025-08-13

Abstract: Quantum-mechanical simulations can offer atomic-level insights into chemical processes on surfaces that are crucial to advancing applications in heterogeneous catalysis, energy storage and greenhouse gas sequestration. Unfortunately, achieving the accuracy needed for reliable predictions has proven challenging. Density functional theory, widely used for its efficiency, can be inconsistent, necessitating accurate methods from correlated wavefunction theory. But high computational demands and substantial user intervention have traditionally made correlated wavefunction theory impractical to carry out for surfaces. Here we present an automated framework that leverages multilevel embedding approaches to apply correlated wavefunction theory to the surfaces of ionic materials with computational costs approaching those of density functional theory. With this framework, we reproduce experimental adsorption enthalpies for a diverse set of 19 adsorbate–surface systems. We further resolve debates on the adsorption configuration of several systems, while offering benchmarks to assess density functional theory. This framework is open source, facilitating the routine application of correlated wavefunction theory to complex problems involving the surfaces of ionic materials.

DOI: 10.1038/s41557-025-01884-y

Source: https://www.nature.com/articles/s41557-025-01884-y