在氮化碳上添加Fe3O4将ROS从HO自由基转移到单线态氧,从而增强和选择性消毒作用

IF 4.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
ACS Omega Pub Date : 2025-09-22 DOI:10.1021/acsomega.5c02329
Dany S. Monje, , , D. Fabio Mercado*, , , Isabel Cristina Ortega-Bedoya, , , Gloria Cristina Valencia, , , Sebastián Amaya-Roncancio, , , Darwin Augusto Torres-Ceron, , , Ronald Vargas, , , Elisabeth Restrepo-Parra, , and , Ricardo A. Torres-Palma*, 
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引用次数: 0

摘要

细菌污染在若干情况下对公共卫生构成严重挑战,例如在开发用于生物医学应用的抗菌表面和提供清洁水方面。为了解决这个问题,在目前的工作中,我们将Fe3O4结构域整合到石墨化碳氮化框架(g-C3N4)上。因此,通过控制裸g-C3N4对铁的吸附,合成了一系列铁掺杂纳米复合材料(g-C3N4、g-C3N4-25、g-C3N4-50、g-C3N4-100和g-C3N4-500)。通过透射电子显微镜(TEM)、x射线衍射(XRD)、热重分析(TGA)、动态光散射(DLS)、傅里叶变换红外光谱(FTIR)、z势(PZC)、荧光、电化学阻抗和x射线光电子能谱(XPS)对这些材料进行了严格的表征,证实了Fe3O4纳米颗粒的成功形成和大量表面缺陷的产生。以环丙沙星(1-环丙基-6-氟-4-氧-7-(哌嗪-1-酰基)-喹啉-3-羧酸)为探针化合物进行光催化实验,在紫外-可见照射下,g-C3N4-25材料具有较高的光催化活性。使用化学清除剂的其他测试显示,从裸g-C3N4中的羟基自由基驱动途径转变为铁修饰材料中更具选择性的单线态氧。在室内光照下,g-C3N4-25对大肠杆菌的消毒效果为6.0 log10 CFU/mL,而原始g-C3N4仅为2.8 log10。与Co和cu掺杂类似物的对比实验进一步表明,铁材料具有优异的动力学和ROS产率。最后,将性能最好的Fe-g-C3N4催化剂包埋在海藻酸盐基质中,形成自消毒表面,在连续5个24 h的辐照循环后,大肠杆菌的浓度保持在5.9±0.3 log10 CFU/mL。这些结果将fe掺杂g-C3N4定位为可持续光催化去除污染物和耐用抗菌涂层的通用平台。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Addition of Fe3O4 on Carbon Nitride Moves the ROS Formation from HO Radicals to Singlet Oxygen Leading to an Enhanced and Selective Disinfecting Action

Bacterial contamination poses serious challenges for public health in several scenarios, such as in developing antimicrobial surfaces for biomedical applications and clean water availability. To face this, in the current work we have incorporated Fe3O4 domains onto the graphitic carbon nitride framework (g-C3N4). Therefore, a series of iron-doped nanocomposites (g-C3N4, g-C3N4-25, g-C3N4-50, g-C3N4-100, and g-C3N4-500) were synthesized by controlling the adsorption of Fe on bare g-C3N4. These materials were rigorously characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), dynamic light scattering (DLS), Fourier transform infrared spectroscopy (FTIR), Z-potential (PZC), fluorescence, electrochemical impedance, and X-ray photoelectron spectroscopy (XPS), confirming the successful formation of Fe3O4 nanoparticles and the creation of abundant surface defects. Photocatalytic experiments using ciprofloxacin (1-cyclopropyl-6-fluoro-4-oxo-7-(piperazin-1-yl)-quinoline-3-carboxylic acid) as probe compound, under UV–Vis irradiation, highlighted the g-C3N4-25 material as the one having the higher photocatalytic activity. Additional tests using chemical scavengers showed a shift from hydroxyl-radical-driven pathways in bare g-C3N4 to the more selective singlet-oxygen in the Fe-modified material. E. coli disinfection under indoor light produced a 6.0 log10 CFU/mL reduction with g-C3N4-25, compared to only 2.8 log10 with pristine g-C3N4. Comparative experiments with Co- and Cu-doped analogues further showed superior kinetics and ROS yields of the iron material. Finally, the best-performing Fe-g-C3N4 catalyst was embedded in an alginate matrix to produce a self-disinfecting surface that maintained a 5.9 ± 0.3 log10 CFU/mL decrease in E. coli after five consecutives 24 h irradiation cycles. These results position Fe-doped g-C3N4 as a versatile platform for the sustainable photocatalytic removal of contaminants and durable antimicrobial coatings.

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来源期刊
ACS Omega
ACS Omega Chemical Engineering-General Chemical Engineering
CiteScore
6.60
自引率
4.90%
发文量
3945
审稿时长
2.4 months
期刊介绍: ACS Omega is an open-access global publication for scientific articles that describe new findings in chemistry and interfacing areas of science, without any perceived evaluation of immediate impact.
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