The unprecedented ability of computations to probe atomic-level details of catalytic systems holds immense promise for the fundamentals-based bottom-up design of novel heterogeneous catalysts, which are at the heart of the chemical and energy sectors of industry. Here, we critically analyze recent advances in computational heterogeneous catalysis. First, we will survey the progress in electronic structure methods and atomistic catalyst models employed, which have enabled the catalysis community to build increasingly intricate, realistic, and accurate models of the active sites of supported transition-metal catalysts. We then review developments in microkinetic modeling, specifically mean-field microkinetic models and kinetic Monte Carlo simulations, which bridge the gap between nanoscale computational insights and macroscale experimental kinetics data with increasing fidelity. We finally review the advancements in theoretical methods for accelerating catalyst design and discovery. Throughout the review, we provide ample examples of applications, discuss remaining challenges, and provide our outlook for the near future.

中文翻译：

---

非均相催化的计算方法

探测催化系统原子级细节的计算能力具有空前的能力，这为新型多相催化剂的基于基本原理的自下而上设计提供了巨大希望，这些催化剂是工业化学和能源领域的核心。在这里，我们批判性地分析计算非均相催化的最新进展。首先，我们将调查所采用的电子结构方法和原子催化剂模型的进展，这些方法使催化界能够建立越来越复杂，现实和准确的负载型过渡金属催化剂活性位点模型。然后，我们回顾微动力学模型的发展，特别是平均场微动力学模型和动力学蒙特卡洛模拟，随着保真度的提高，纳米级计算洞察力与宏观实验动力学数据之间的差距得以弥合。最后，我们回顾了加速催化剂设计和发现的理论方法的进展。在整个审查过程中，我们提供了充足的应用示例，讨论了仍然存在的挑战，并提供了近期的展望。