Orbital interaction involving metal cation−π is an important form for electron transfer regulation. To accelerate the interfacial electron transfer of peroxymonosulfate (PMS) activation for water treatment, we report a new strategy through bonding atomically dispersed cobalt with nanospheric C-based graphene-like structures (SACo-NGs) to form metal cation−π structure, driving rapid and directional transfer of the electrons of pollutants to PMS on the catalyst surface. The catalyst SACo-NGs is synthesized by an enhanced hydrothermal-sintering method and the formation of metal cation−π structure is demonstrated by X-ray absorption fine structure (EXAFS), X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance spectroscopy (EPR) and Raman spectroscopy. It is found that Co−π structures (Co²⁺-N-C_π) play a key role for the efficient activation of PMS, which results in pollutants being greatly removed in a few minutes. During the reaction, pollutants can donate electrons for the system through π−π interaction accompanying by the direct oxidative degradation of pollutants. The obtained electrons are quickly transferred to the atomically dispersed cobalt sites through the formed cation−π structure, which promotes the activation of PMS. This is a successful practice in the field of PMS activation using cation−π structure to accelerate electron transfer and achieve rapid degradation of pollutants.

涉及金属阳离子-π的轨道相互作用是电子转移调节的重要形式。为了加快过氧单硫酸盐（PMS）活化的界面电子转移以进行水处理，我们报告了一种新的策略，该方法通过将原子分散的钴与纳米球形C基石墨烯样结构（SACo-NGs）结合以形成金属阳离子-π结构，从而迅速发展以及污染物电子向催化剂表面PMS的定向转移。通过增强水热烧结法合成了催化剂SACo-NGs，并通过X射线吸收精细结构（EXAFS），X射线光电子能谱（XPS），电子顺磁共振光谱（ EPR）和拉曼光谱。发现Co-π结构（Co ²⁺ -NC_π）在有效激活PMS中起着关键作用，这导致污染物在几分钟内被大量清除。在反应过程中，污染物可以通过π-π相互作用（伴随污染物的直接氧化降解）为系统贡献电子。获得的电子通过形成的阳离子-π结构快速转移到原子分散的钴位点，从而促进PMS的活化。这是在使用阳离子-π结构的PMS激活领域加速电子转移并实现污染物快速降解的成功实践。