Huang Yihan, Zhang Jiali, Guo Zhuang, Zang Haochun, Zheng Maosheng, Hao Tong, Wei Jian
Key Laboratory of Resources and Environmental Systems Optimization, Ministry of Education, College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, China; State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China.
State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China.
Environ Res. 2025 Apr 1;270:121013. doi: 10.1016/j.envres.2025.121013. Epub 2025 Jan 31.
This study aimed to synthesize a bimetallic Fe-Mo modified N-doped carbon material (FeMo@NCN) using a simple pyrolysis method. Structural and physical characterizations confirmed the successful incorporation of Fe and Mo into the catalyst. The FeMo@NCN/PMS system exhibited an excellent acetaminophen (ACE) degradation rate (k = 0.1232 min), which is 51 times higher than that of NCN/PMS system (k = 0.0024 min). Mechanistic analysis revealed that the Fe/Mo interaction, as well as the synergistic effects between Mo-N and Fe-N sites, facilitated the continuous generation of reactive oxygen species (ROS), including SO and •OH. Specifically, Mo doping to promoted the regeneration of Fe, contributing to the recovery of catalytic activity and playing a key role in maintaining high degradation efficiency. Furthermore, electrochemical analysis demonstrated that the Fe and Mo doping significantly enhanced the electronic transfer properties of the material, revealing the existence of an electron transfer-based non-radical pathway. Additionally, FeMo@NCN exhibited remarkable stability across a wide pH range (3-9). The intermediate degradation products and degradation pathways of ACE were identified, and the toxicity of ACE and its degradation products were evaluated. This work provides new insights into improving the performance of carbon-based materials for efficient removal of refractory organic compounds in PMS systems.
本研究旨在采用简单的热解方法合成一种双金属铁-钼改性的氮掺杂碳材料（FeMo@NCN）。结构和物理表征证实了铁和钼成功掺入催化剂中。FeMo@NCN/PMS体系表现出优异的对乙酰氨基酚（ACE）降解速率（k = 0.1232 min⁻¹），比NCN/PMS体系（k = 0.0024 min⁻¹）高51倍。机理分析表明，铁/钼相互作用以及钼-氮和铁-氮位点之间的协同效应促进了包括硫酸根自由基（SO₄•⁻）和羟基自由基（•OH）在内的活性氧物种（ROS）的持续产生。具体而言，钼的掺杂促进了铁的再生，有助于催化活性的恢复，并在维持高降解效率方面发挥关键作用。此外，电化学分析表明，铁和钼的掺杂显著增强了材料的电子转移性能，揭示了基于电子转移的非自由基途径的存在。此外，FeMo@NCN在较宽的pH范围（3 - 9）内表现出显著的稳定性。确定了ACE的中间降解产物和降解途径，并评估了ACE及其降解产物的毒性。这项工作为提高基于碳的材料在PMS体系中高效去除难降解有机化合物的性能提供了新的见解。
