3D porous Co₃O₄/nitrogen-doped graphene aerogel (NGA) hybrid for heterogeneous activation of peroxymonosulfate (PMS) was prepared by feasible hydrothermal and freeze-drying methods. The morphology, crystal structure and chemical composition of the catalyst were investigated by scanning electron microscopy, X-ray diffractometer, X-ray photoelectron spectroscopy, Raman spectra and Fourier transform infrared spectroscopy. Co₃O₄/NGA at a high N doping level of 7.6% (in atomic percentage) exhibited excellent catalytic performance for acid orange 7 (AO7) degradation, with almost complete removal within 30 min. Moderate PMS content, higher temperature and lower solution pH conditions would facilitate the decomposition of AO7. The catalyst possesses excellent long-term stability and recycling performance with simple separation and post-treatment approaches. Kinetic models was developed to simulate the transformation of main active radical species and the AO7 oxidation profiles, considering effects of coexisting ions (Cl⁻ and HCO₃⁻). Based on results of electron spin resonance, typical quenching tests and kinetic calculation, sulfate radicals play dominate role in AO7 degradation. Co₃O₄ nanocrystals and the new active sites created by nitrogen doping into graphene honeycomb network should synergistically contribute to the high degradation efficiency. This work has expanded the possibility of recyclable catalysts design for heterogeneous activation of PMS, with a dual catalytically active center and desirable stability.

通过可行的水热和冷冻干燥方法，制备了用于过氧化单硫酸盐（PMS）异质活化的3D多孔Co ₃ O ₄ /氮掺杂石墨烯气凝胶（NGA）杂化物。通过扫描电子显微镜，X射线衍射仪，X射线光电子能谱，拉曼光谱和傅里叶变换红外光谱对催化剂的形貌，晶体结构和化学组成进行了研究。钴₃ O ₄高氮掺杂水平（原子百分数）为/ NGA时，其对酸性橙7（AO7）降解表现出出色的催化性能，在30分钟内几乎被完全去除。适中的PMS含量，较高的温度和较低的溶液pH条件将促进AO7的分解。该催化剂具有优异的长期稳定性和再循环性能，具有简单的分离和后处理方法。动力学模型的开发是为了模拟主要活性自由基及氧化AO7型材改造，考虑到共存离子的影响（CL ^-和HCO ₃ ^- ）。根据电子自旋共振的结果，典型的猝灭测试和动力学计算，硫酸根在AO7降解中起主要作用。钴₃O ₄纳米晶体和氮掺杂到石墨烯蜂窝网络中产生的新的活性位点应协同促进高降解效率。这项工作扩大了具有双催化活性中心和所需稳定性的PMS异相活化的可回收催化剂设计的可能性。