We provide a critical overview of progress and challenges in computationally modeling multistep reaction mechanisms relevant for catalysis and electrocatalysis. We first discuss how the chemical and materials space of energetically efficient catalysis can be explored with computational chemistry. Since reactions for renewable energy catalysis can involve acid–base chemistry and/or ions under aqueous conditions, we then summarize how solvation can be modeled with quantum chemistry schemes using implicit, mixed implicit/explicit, and fully explicit solvation modeling. We will discuss the insights (and limitations) of these solvation models primarily through the scope of understanding CO₂ reduction reaction mechanisms, but these will also be applicable for future work elucidating other reaction mechanisms of critical importance for human sustainability such as H₂O oxidation and N₂ reduction.

中文翻译：

---

在建模可再生燃料和化学溶剂化反应机理方面的进展和挑战

我们提供了对与催化和电催化相关的多步反应机理进行计算建模的进展和挑战的重要概述。我们首先讨论如何利用计算化学来探索能效催化的化学和材料空间。由于可再生能源催化的反应可能涉及在水性条件下的酸碱化学和/或离子，因此我们总结了如何使用隐式，混合隐式/显式和完全显式溶剂化模型通过量子化学方案对溶剂化进行建模。我们将主要通过了解CO ₂的范围来讨论这些溶剂化模型的见解（和局限性）。还原反应机理，但是这些也将适用于将来的工作，阐明对人类可持续性至关重要的其他反应机理，例如H ₂ O氧化和N ₂还原。