Two coordination structures (Co-N₄ or Co-N₃) of cobalt single-atom catalysts (Co-SACs) were prepared by using the chitosan as starting precursor to evaluate the modulated coordination microenvironment of Co-SACs for organics degradation. The degradation performances for carbamazepine (CBZ) as well as the radical/nonradical pathways in Co-N₄/PMS and Co-N₃/PMS systems was evaluated. Results showed that more radicals could be produced by the Co-N₃ catalyst via stronger PMS adsorption as well as the subsequent peroxide bond cleavage of PMS. In addition, a lower energy gap between the CBZ and Co-N₃/PMS complex was endowed for the Co-N₃ coordination to boost stronger electron-transfer process for CBZ. As a result, both radical and electron-transfer process was boosted by the coordinated Co-N₃ sites than those of Co-N₄ coordination. This work provides a new insight on the versatile catalytic pathways with modulated coordination microenvironment of carbon-based SACs for high-efficiency PMS activation.

以壳聚糖为起始前驱体，制备了钴单原子催化剂（Co-SACs）的两种配位结构（Co-N 4 或Co _- N _{3 ），以评估Co-SACs调节的配位微环境对有机物降解的影响。}评估了卡马西平 (CBZ) 的降解性能以及 Co-N ₄ /PMS 和 Co-N _{3 /PMS 系统中的自由基/非自由基途径。结果表明，Co-N 3}催化剂可以通过更强的 PMS 吸附以及随后的 PMS 过氧化物键断裂产生更多的自由基。此外，CBZ 和 Co-N ₃ /PMS 复合物之间的能隙较低，赋予 Co-N ₃协调以促进 CBZ 更强的电子转移过程。结果，与Co-N ₄配位相比，配位Co-N ₃位点促进了自由基和电子转移过程。这项工作为具有碳基 SAC 的调制配位微环境的多功能催化途径提供了新的见解，以实现高效 PMS 激活。