Tailoring the interfacial reaction pathway and low consumption strategy for the high efficiency Fenton-like processes is environmentally desirable but still challenging. Herein, single Co atom-doped g-C₃N₄ was prepared for peroxymonosulfate (PMS) activation to reveal the interfacial reaction of high-valent cobalt-oxo species [Co(IV) = O] to singlet oxygen (¹O₂) and construct an energy efficient Fenton-like system. Experimental results showed that the system could achieve 99.6% carbamazepine removal with k_obs of 0.355 min⁻¹, while the decomposition of PMS was mild (0.0988 and 0.00917 min⁻¹ in 0–2 and 2–30 min, respectively). Mechanistic studies revealed the reaction of Co(IV) = O to ¹O₂, which moderated the reduction of Co sites, thus slowing the decomposition rate of PMS. But the synergistic effect of ¹O₂ and Co(IV) = O maintained the high activity of the system. Combined with first-principles calculations, the optimal evolution path of PMS was PMS → OH*→Co(IV) = O → OO*→¹O₂, accompanied by the Co(II)/Co(III)/Co(IV) redox cycle. The work proposed a new interfacial reaction in term of Co(IV) = O triggered ¹O₂ generation, resulting in the construction of an energy-efficient Fenton-like system and provided a novel idea for the development of efficient and low consumption water purification technology.

为高效的类芬顿过程定制界面反应途径和低消耗策略在环境上是可取的，但仍然具有挑战性。在此，制备了单 Co 原子掺杂的 gC ₃ N ₄用于过一硫酸盐 (PMS) 活化，以揭示高价钴氧物种 [Co(IV) = O] 与单线态氧 ( ¹ O ₂ ) 的界面反应并构建一种节能的类芬顿系统。实验结果表明，该系统对卡马西平的去除率达到99.6%，k _obs为0.355 min ⁻¹，而PMS的分解程度较轻（0.0988和0.00917 min ^{−1 ）}分别在 0-2 分钟和 2-30 分钟内）。^{机理研究揭示了Co(IV) = O到1} O ₂的反应，减缓了Co位点的还原，从而减缓了PMS的分解速率。^但1 O ₂和Co(IV) = O的协同作用维持了体系的高活性。结合第一性原理计算，PMS的最优演化路径为PMS → OH*→Co(IV) = O → OO*→ ¹ O ₂，​​并伴有Co(II)/Co(III)/Co(IV)氧化还原循环。该工作提出了一种新的界面反应，即 Co(IV) = O 引发的¹ O ₂产生了高效节能的类芬顿系统，为开发高效低耗的净水技术提供了新的思路。