School of Environment and Energy, South China University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006, China; The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, Guangzhou Higher Education Mega Centre, Guangzhou 510006, China.
School of Environment and Energy, South China University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006, China; The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, Guangzhou Higher Education Mega Centre, Guangzhou 510006, China; Guangdong Engineering and Technology Research Center for Environmental Nanomaterials, Guangzhou 510006, China.
J Hazard Mater. 2023 Jan 15;442:130016. doi: 10.1016/j.jhazmat.2022.130016. Epub 2022 Sep 23.
To address the difficulty of precisely regulating the two-electron oxygen reduction reaction (2e-ORR) and investigate the synergistic effect of hydrogen peroxide (HO) and peroxymonosulfate (PMS), a heterogeneous electro-catalyst was synthesized via carbonation of boron (B) and sulfur (S) co-doping electrospun nanofibers containing iron and cobalt (B, S-Fe/Co@C-NCNFs-900), and used to degrade levofloxacin (Levo) in the electro-activating PMS with self-made cathode material (E-cathode-PMS) system. The morphological, structural, and electrochemical characteristics have been investigated. The results showed that B and S co-doping could remarkably enhance electron transfer and manage two-electron oxygen reduction, which was more favorable for HO generation. Levo degradation efficiency could reach 99.63% with a reaction rate of 0.3056 min in 20 min under the appropriate conditions (pH = 4, current = 20 mA, and [PMS] = 8.0 mM). The steady-state concentration of singlet oxygen (O) was calculated to be 669.17 × 10 M, which was 15.42, 29.74, and 45.00 times respectively than that of HO·/O· (43.40 × 10 M), ·OH (22.25 × 10 M) and SO·(14.87 × 10 M), signifying that O was the predominant reactive oxygen species (ROS) involved in Levo removal. The high TOC removal (74.19%), low energy consumption (0.14 kWh m order), few intermediates toxicity, and excellent Levo degradation efficiency for complex wastewater with various anions and matrixes showed the prospective practical applications of the E-cathode-PMS system. Overall, this study provides a useful strategy to regulate and control the 2e-ORR pathway.
为了解决精确调控两电子氧还原反应(2e-ORR)的难题,并研究过氧化氢(HO)和过一硫酸盐(PMS)的协同作用,通过碳化硼(B)和硫(S)共掺杂含有铁和钴的电纺纳米纤维(B、S-Fe/Co@C-NCNFs-900)合成了一种非均相电催化剂,并用于在自制阴极材料(E-阴极-PMS)系统中电激活过一硫酸盐降解左氧氟沙星(Levo)。研究了其形态、结构和电化学特性。结果表明,B 和 S 共掺杂可以显著增强电子转移并管理两电子氧还原,更有利于 HO 的生成。在适当的条件下(pH = 4、电流 = 20 mA 和 [PMS] = 8.0 mM),20 min 内 Levo 降解效率可达 99.63%,反应速率为 0.3056 min。计算得到单线态氧(O)的稳态浓度为 669.17 × 10 M,分别是 HO·/O·(43.40 × 10 M)、·OH(22.25 × 10 M)和 SO·(14.87 × 10 M)的 15.42、29.74 和 45.00 倍,表明 O 是参与 Levo 去除的主要活性氧物种(ROS)。高 TOC 去除率(74.19%)、低能耗(0.14 kWh m 级)、中间产物毒性低以及对各种阴离子和基质复杂废水的优异 Levo 降解效率,显示出 E-阴极-PMS 系统具有广阔的实际应用前景。总的来说,本研究为调控 2e-ORR 途径提供了一种有用的策略。