【摘要】 为实现含能材料行业产生的N,N-二甲基甲酰胺（DMF）废液的高效无害化处理，采用催化超临界水氧化（CSCWO）技术，系统探究了反应温度、压力、过氧系数及催化剂对DMF降解效果的影响。结果表明，温度是影响化学需氧量（COD）与氨氮（NH₃-N）降解的最关键因素。通过正交实验优化，获得COD降解的最佳条件为530℃、25 MPa、过氧系数0.2，而NH₃-N的深度氧化则需更高的氧环境。在非催化条件下，NH₃-N作为难降解中间产物易大量积累。引入CeO₂催化剂后，凭借其优异的储释氧能力与表面氧空位，显著促进了羟基（·OH）自由基的生成与NH₃-N向N₂的定向转化，其催化性能显著优于CuO、MnO₂与Fe₂O₃。最终，通过构建“足够反应时间（34 s）-CeO₂催化-充足氧化剂（n=2.5）”的协同反应体系，在500℃、21 MPa条件下实现了COD接近完全矿化（降解率≥99%），出水氨氮质量浓度降至25 mg·L^-1。这证实了超临界水氧化（SCWO）技术协同CeO₂催化可有效解决DMF废液处理中氨氮深度氧化的技术难题，为高浓度含氮有机废液的治理提供了可靠路径。更多还原

【Abstract】 To achieve efficient and harmless treatment of N,N-dimethylformamide（DMF） wastewater generated in the energetic materials industry, catalytic supercritical water oxidation（CSCWO） technology was employed to systematically investigate the effects of reaction temperature, pressure, oxidant ratio, and catalyst on DMF degradation. The results indicated that temperature was the most critical factor affecting the degradation of chemical oxygen demand（COD） and ammonia nitrogen（NH₃-N）. Through orthogonal experimental optimization, the optimal conditions for COD degradation were found to be 530 ℃, 25 MPa, and oxidant ratio of 0.2, while deeper oxidation of NH₃-N required higher oxygen environment. Under non-catalytic conditions, NH₃-N as a difficult-to-degrade intermediate, tended to accumulate significantly. With the introduction of the CeO₂ catalyst, its excellent oxygen storage-release capacity and surface oxygen vacancies significantly promoted the generation of hydroxyl（·OH） radicals and the targeted conversion of NH₃-N to N₂, with catalytic performance significantly superior to CuO, MnO₂, and Fe₂O₃. Finally, by constructing a synergistic reaction system of "sufficient reaction time（34 s）-CeO₂ catalysis-sufficient oxidant（n=2.5）," under conditions of 500 ℃ and 21 MPa, COD was nearly completely mineralized（degradation rate ≥99%） and the effluent ammonia nitrogen mass concentration was reduced to 25 mg·L^-1. This confirmed that supercritical water oxidation（SCWO） combined with CeO₂ catalysis can effectively address the technical challenge of deep oxidation of ammonia nitrogen in DMF wastewater treatment, providing a reliable approach for the treatment of high-concentration nitrogencontaining organic wastewater.更多还原