Hubei Key Laboratory of Mineral Resources Processing and Environment, School of Resources and Environmental Engineering, Wuhan University of Technology, Wuhan 430070, China.
Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, PR China.
Sci Total Environ. 2023 Feb 10;859(Pt 1):160001. doi: 10.1016/j.scitotenv.2022.160001. Epub 2022 Nov 8.
Highly efficient and stable heterogeneous catalysts were desired to activate periodate (PI) for sustainable pollution control. Herein, iron-nitrogen-carbon catalyst was synthesized using a facile molten-salts mediated pyrolysis strategy (denoted as FeNC-MS) and employed to activate PI for the degradation of acetaminophen (ACE). Compared with iron-nitrogen-carbon catalyst prepared by direct pyrolysis method (marked as FeNC), FeNC-MS exhibited superior catalytic activity due to its large specific surface area (1600 m g) and the abundance of FeN sites. The batch experiments revealed that FeNC/PI process achieved 37 % ACE removal within 20 min, while ACE removal in FeNC-MS/PI process was 98 % under the identical conditions. Integrated with electron paramagnetic resonance tests, quenching experiments, chemical probe identification, and electrochemical experiments, we demonstrated that FeNC-MS-PI complexes-mediated electron transfer was the predominant mechanism for the oxidation of ACE. Further analysis disclosed that FeN sites in FeNC-MS were the main active sites for the activation of PI. Additionally, FeNC-MS/PI process exhibited significant resistance to humic acid and background electrolyte, and avoided the secondary pollution imposed by Fe leaching. The possible degradation pathways of ACE were proposed. The germination experiments of lettuce seeds showed that the ecotoxicity of ACE solution was significantly reduced after treatment with FeNC-MS/PI process. Overall, this study provided a facile strategy for the synthesis of efficient iron-nitrogen-carbon catalysts and gained fundamental insight into the mechanism of PI activation by iron-nitrogen-carbon catalysts for pollutants degradation.
高效稳定的多相催化剂被期望能激活高碘酸盐(PI)以实现可持续的污染控制。本文采用简便的熔融盐介导热解法(记为 FeNC-MS)合成了铁氮碳催化剂,并将其用于激活 PI 以降解扑热息痛(ACE)。与直接热解法制备的铁氮碳催化剂(记为 FeNC)相比,由于其较大的比表面积(1600 m g)和丰富的 FeN 位,FeNC-MS 表现出更高的催化活性。批实验表明,FeNC/PI 体系在 20 min 内可实现 37%的 ACE 去除率,而在相同条件下,FeNC-MS/PI 体系中 ACE 的去除率高达 98%。结合电子顺磁共振测试、猝灭实验、化学探针鉴定和电化学实验,我们证明了 FeNC-MS-PI 复合物介导的电子转移是 ACE 氧化的主要机制。进一步分析表明,FeNC-MS 中的 FeN 位是激活 PI 的主要活性位。此外,FeNC-MS/PI 体系对腐殖酸和背景电解质具有显著的抵抗力,并避免了 Fe 浸出带来的二次污染。提出了 ACE 的可能降解途径。生菜种子发芽实验表明,FeNC-MS/PI 体系处理后 ACE 溶液的生态毒性显著降低。总之,本研究为高效铁氮碳催化剂的合成提供了一种简便的策略,并深入了解了铁氮碳催化剂激活 PI 用于污染物降解的机制。