Increasing the number of electroactive sites to enhance catalytic activity is by far the best approach for enhancing the oxygen reduction reaction; however, the development of a catalyst with high electrochemical performance and long-term stability remains a significant challenge because of the weak binding energy of oxygenated species. Herein, we report the fabrication of an extended Ag nanoparticle network on a defect-rich carbon nanotube (CNT) ternary composite, CNT@pPPD-Ag, derived from polyparaphenylenediamine (pPPD) with a porous crystalline framework that enhances the edge-rich N-species-decorated carbon nanotubes. The N-bridged-polymer/CNT composite facilitates the aligned dispersion of Ag nanoparticles anchored at the low coordination sites, increases the surface area and pore size volume, and exposes effective CNT–N–Ag active sites for enhanced oxygen absorption to convert O₂ into H₂O. In addition, the reduced electron delocalization around the Ag atoms due to the N-species enhances the charge interaction between the neighboring N and Ag atoms, leading to the strengthening of the interaction with the adsorbed oxygen species, thereby increasing the intrinsic activity of each electroactive site. In this work, CNT@pPPD-Ag composite explored with remarkable low onset potential (-0.041 V) and limiting current density (-5.80 mA cm⁻²) in an alkaline environment, and far exceeds the performance of expensive Pt/C catalysts.

增加电活性位点的数量以增强催化活性是迄今为止增强氧还原反应的最佳方法；然而，由于含氧物质的结合能较弱，因此开发具有高电化学性能和长期稳定性的催化剂仍然是一个重大挑战。在此，我们报告了在富含缺陷的碳纳米管 (CNT) 三元复合材料 CNT@pPPD-Ag 上制造扩展的 Ag 纳米颗粒网络，该复合材料源自聚对苯二胺 (pPPD)，具有多孔结晶框架，可增强富边缘 N-物种修饰的碳纳米管。N-桥接聚合物/碳纳米管复合材料促进了固定在低配位点的银纳米粒子的定向分散，增加了表面积和孔径体积，₂转化为 H ₂ O。此外，由于 N 物种导致 Ag 原子周围的电子离域减少增强了相邻 N 和 Ag 原子之间的电荷相互作用，导致与吸附氧物种的相互作用加强，从而增加每个电活性位点的内在活性。在这项工作中，CNT@pPPD-Ag 复合材料在碱性环境中具有显着的低起始电位 (-0.041 V) 和极限电流密度 (-5.80 mA cm ^-2 )，远远超过昂贵的 Pt/C 催化剂的性能。