Single-atom catalysts (SACs) have attracted considerable research interest owing to their combined merits of homogeneous and heterogeneous catalysts. However, the uniform and isolated active sites of SACs fall short in catalysing complex chemical processes that simultaneously involve multiple intermediates. In this Review, we highlight an emerging class of catalysts with adjacent binary active centres, which is called integrative catalytic pairs (ICPs), showing not only atomic-scale site-to-site electronic interactions but also synergistic catalytic effects. Compared with SACs or their derivative dual-atom catalysts (DACs), multi-interactive intermediates on ICPs can overcome kinetic barriers, adjust reaction pathways and break the universal linear scaling relations as the smallest active units. Starting from this active-site design principle, each single active atom can be considered as a brick to further build integrative catalytic clusters (ICCs) with desirable configurations, towards trimer or even larger multi-atom units depending on the requirement of a given reaction.

单原子催化剂 （SAC） 因其均相和非均相催化剂的综合优点而引起了相当大的研究兴趣。然而，SAC 的均匀和分离活性位点在催化同时涉及多个中间体的复杂化学过程方面存在不足。在这篇综述中，我们重点介绍了一类具有相邻二元活性中心的新兴催化剂，称为整合催化对 （ICP），不仅显示出原子尺度的位点间电子相互作用，还显示出协同催化效应。与 SACs 或其衍生物双原子催化剂 （DACs） 相比，ICP 上的多相互作用中间体可以作为最小的活性单元克服动力学障碍、调整反应途径并打破通用线性缩放关系。从这种活性位点设计原理出发，每个单个活性原子都可以被视为一块砖，以进一步构建具有所需配置的整合催化簇 （ICC），具体取决于给定反应的要求，朝着三聚体甚至更大的多原子单元发展。