Heterogeneous electrocatalysis is critical to many energy conversion processes. Theoretical and computational approaches are essential to interpret experimental data and provide the mechanistic understanding necessary to design more effective catalysts. However, automated general procedures to build predictive theoretical and computational frameworks are not readily available; specific choices must be made in terms of the atomistic structural model and the level of theory, as well as the experimental data used to inform and validate these choices. Here we outline some best practices for modelling heterogeneous systems and present examples in the context of catalysis at metal electrodes and oxides. The level of theory should be chosen for the specific system and properties of interest, and experimental validation is essential from the beginning to the end of the study. Continuous feedback and ultimate integration between experiment and theory enhances the power of calculations to elucidate mechanisms, identify effective descriptors and clarify design principles.

多相电催化对于许多能量转换过程至关重要。理论和计算方法对于解释实验数据和提供设计更有效催化剂所需的机械理解至关重要。然而，构建预测性理论和计算框架的自动化通用程序并不容易获得；必须在原子结构模型和理论水平以及用于告知和验证这些选择的实验数据方面做出具体选择。在这里，我们概述了建模异质系统的一些最佳实践，并在金属电极和氧化物催化的背景下提供了示例。应该为特定的系统和感兴趣的属性选择理论水平，从研究开始到结束，实验验证都是必不可少的。实验与理论之间的持续反馈和最终整合增强了计算能力，以阐明机制、确定有效的描述符并阐明设计原则。