Development of a new catalytic system with synergistic multiple active sites to effectively promote the activation of peroxymonosulfate (PMS) is crucial for the control of emerging organic pollutants in water, but it is still challenging. Herein, we explore robust CoP_x-implanted porous N-doped carbon frameworks (CoP_x@NC) to effectively activate PMS and eliminate tetracycline (TC). The cobalt phosphides in CoP_x@NC spontaneously create the distinctive charge imbalance to form asymmetrically charged Co^δ+ and P^δ− as dual active sites to efficiently enhance catalytic activity, while the positively polarized carbon induced by neighboring electronegative N atoms in CoP_x@NC contributes to high catalytic efficiency in parallel. As an advanced catalyst, CoP_x@NC displays excellent catalytic performances in PMS activation toward efficient TC degradation with an improved rate constant of 0.137 min⁻¹ and a favorable k-value of 1.43 μmol s⁻¹ g⁻¹. Mechanistic analysis clearly unveils that the non-radical pathway (singlet oxygen ¹O₂ and direct electron transfer) in CoP_x@NC/PMS system dominantly governs the TC degradation along with cooperative radical (SO₄^·− and ·OH) pathway. This study enriches the charge imbalance strategy for catalyst design and highlights a new catalytic platform to activate PMS for efficient pollutant degradation in water.

开发具有协同多个活性位点的新型催化系统以有效促进过一硫酸盐（PMS）的活化对于控制水中新兴有机污染物至关重要，但仍然具有挑战性。在此，我们探索了坚固的 CoP _x植入多孔 N 掺杂碳框架 (CoP _x @NC)，以有效激活 PMS 并消除四环素 (TC)。_{CoP x} @NC中的磷化钴自发地产生独特的电荷不平衡，形成带不对称电荷的 Co ^δ+和 P ^{δ−作为双活性位点，有效增强催化活性，而 CoP} _x中邻近电负性 N 原子诱导正极化的碳@NC 有助于并行提高催化效率。作为一种先进的催化剂，CoP _x @NC 在 PMS 活化和有效 TC 降解方面表现出优异的催化性能，速率常数提高到 0.137 min ^-1，k 值达到 1.43 μmol s ^-1 g ^-1。机理分析清楚地揭示了CoP _x @NC/PMS 系统中的非自由基途径（单线态氧¹ O ₂和直接电子转移）与协同自由基 (SO ₄ ^·−和·OH)途径。这项研究丰富了催化剂设计的电荷不平衡策略，并突出了一个新的催化平台来激活 PMS 以有效降解水中的污染物。