Single-atom catalysts (SACs), among which nitrogen-doped graphene-supported SACs are successful models, have been extensively investigated for electrocatalysts. Although oxygen is a common impurity in graphene, metal-oxygen-based SACs are unutilized. Here, we devise a new type of oxygen-coordinated SAC (M-O-C) with a computation-aided approach. Theoretical modeling predicts that the metal atoms are strongly immobilized by carbonyl ligands in unzipped carbon nanotubes, and then the Ni-O-C SAC is synthesized for the oxygen evolution reaction (OER). It shows excellent OER activity with a low overpotential (228/325 mV at 10/100 mA cm⁻²), small Tafel slope (36 mV per decade), and long-term durability over 150 h. We find that the highly electronegative oxygen ligand deviates from the conventional linear scaling relationship by shifting toward a more reactive region, so the inductive effect of the oxygen ligand leads to superior OER activity. This “theory first followed by experiment” strategy would help in the design of various SACs.

单原子催化剂（SAC），其中氮掺杂石墨烯负载的 SAC 是成功的模型，已被广泛研究用于电催化剂。尽管氧是石墨烯中的常见杂质，但基于金属氧的 SAC 尚未得到利用。在这里，我们采用计算辅助方法设计了一种新型的氧配位 SAC (MOC)。理论模型预测，金属原子被羰基配体牢固地固定在未压缩的碳纳米管中，然后合成 Ni-OC SAC 用于析氧反应 (OER)。它表现出优异的OER活性，具有低过电位（10/100 mA cm ^{-2时为228/325 mV} ）、小塔菲尔斜率（每十年36 mV）和超过150小时的长期耐久性。我们发现，高电负性氧配体通过向更具反应性的区域移动而偏离了传统的线性比例关系，因此氧配体的诱导效应导致了优异的OER活性。这种“先理论后实验”的策略将有助于设计各种 SAC。