Yang Fencheng, Jiang Guodong, Chang Qing, Huang Peipei, Lei Ming
Key Laboratory of Catalysis and Materials Science of Hubei Province, College of Resources and Environmental Science, South-Central University for Nationalities, Wuhan, 430074, Hubei, China.
College of Chemistry and Chemical Engineering, Hubei Collaborative Innovation Center for High Efficient Utilization of Solar Energy, Hubei University of Technology, Wuhan, 430074, Hubei, China.
Chemosphere. 2021 Nov;283:131154. doi: 10.1016/j.chemosphere.2021.131154. Epub 2021 Jun 11.
Fe/N-doped carbon magnetic nanocubes (Fe/N-C MNCs) were feasibly fabricated through in situ thermal transformations of Prussian blue nanocubes (PB NCs) in an inert atmosphere, and the resultant composite employed as the heterogeneous noble-metal-free catalyst possessed satisfactory catalytic performance in hydrogen peroxide activation. By examining the properties of Fe/N-C MNCs, we demonstrate for the first time that the catalyst could act in synergy with ultrasonic irradiation and accelerate the selectivity of the degradation reaction of dyes. The degradation efficiency of the organic positively charged dye (methylene blue) is significantly increased after ultrasonic irradiation addition, probably owing to charge matching between a positively charged dye and the Fe/N-C MNCs. Interestingly, organic pollution degradation mainly follows a non-radical pathway. Furthermore, singlet oxygen (O) is predominantly produced by Fe/N-C MNCs on HO activation, and it is the contributor to catalytic degradation instead of hydroxyl and/or superoxide anion radicals. Moreover, the Fe/N-C MNCs exhibit excellent stability and reusability. These findings offer interesting insights into the potential application of functional noble-metal-free materials in catalysis and wastewater remediation under ultrasonic radiation.
通过在惰性气氛中原位热转化普鲁士蓝纳米立方体(PB NCs),成功制备了铁/氮掺杂碳磁性纳米立方体(Fe/N-C MNCs),所得复合材料作为非均相无贵金属催化剂,在过氧化氢活化方面具有令人满意的催化性能。通过研究Fe/N-C MNCs的性质,我们首次证明该催化剂可与超声辐射协同作用,加速染料降解反应的选择性。添加超声辐射后,有机带正电荷染料(亚甲基蓝)的降解效率显著提高,这可能是由于带正电荷的染料与Fe/N-C MNCs之间的电荷匹配。有趣的是,有机污染物降解主要遵循非自由基途径。此外,Fe/N-C MNCs在过氧化氢活化时主要产生单线态氧(O),它是催化降解的贡献者,而非羟基和/或超氧阴离子自由基。而且,Fe/N-C MNCs表现出优异的稳定性和可重复使用性。这些发现为功能性无贵金属材料在超声辐射下的催化和废水修复中的潜在应用提供了有趣的见解。