Two atomically dispersed cobalt catalysts with different nitrogen coordination numbers (denoted as Co_SA-N_x-C) were synthesized and firstly compared to activate peroxydisulfate (PDS) for bisphenol A (BPA) degradation. Theoretical calculations unveiled that lowering the CoN coordination number from four to three can apparently increase the electron density of the single Co atom in Co_SA-N₃-C to enhance PDS conversion. The low-coordinated Co_SA-N₃-C with CoN₃ coordination structure displays a high specific activity of 0.067 L min¹ m², which is 1.31 times greater than that of Co_SA-N₄-C with normal CoN₄ configuration (0.051 L min¹ m²) in PDS activation. Electron paramagnetic resonance (EPR) measurements and quenching tests confirmed the primary role of sulfate radical (SO₄^•−) in BPA oxidation over Co_SA-N₃-C with PDS. Moreover, Co_SA-N₃-C delivers favorable durability for PDS activation and potential practicability for realistic wastewater remediation. These findings provide a novel and useful avenue to coordination number modulation of SACs for wider environmental applications.

合成了两种具有不同氮配位数的原子分散钴催化剂（表示为 Co _SA -N _x -C），并首先比较活化过二硫酸盐 (PDS) 对双酚 A (BPA) 的降解。理论计算表明，将 Co N 配位数从 4降低到 3 可以明显增加 Co _SA -N ₃ -C 中单个 Co 原子的电子密度，从而增强 PDS 转换。具有Co N ₃配位结构的低配位Co _SA -N ₃ -C显示出0.067 L min ¹ m ²的高比活度，是Co的1.31倍_SA -N ₄ -C在 PDS 活化中具有正常的 Co N ₄配置（0.051 L min ¹ m ²）。电子顺磁共振 (EPR) 测量和猝灭测试证实了硫酸根 (SO ₄ ^•- ) 在使用 PDS 的Co _SA -N ₃ -C 上的BPA 氧化中的主要作用。此外，Co _SA -N ₃ -C 为 PDS 活化提供了良好的耐久性和现实废水修复的潜在实用性。这些发现为 SAC 的配位数调制提供了一种新颖且有用的途径，以用于更广泛的环境应用。