Liu Zhen, Chen Renyu, Li Mengyu, Yang Shanshan, Zhang Jiang, Yuan Shaochun, Hou Yizhi, Li Cong, Chen Yao
School of River and Ocean Engineering, Chongqing Jiaotong University, Chongqing 400074, China; Key Laboratory of Hydraulic and Waterway Engineering of the Ministry of Education, Chongqing Jiaotong University, Chongqing 400074, China.
School of River and Ocean Engineering, Chongqing Jiaotong University, Chongqing 400074, China.
J Hazard Mater. 2023 Oct 5;459:132089. doi: 10.1016/j.jhazmat.2023.132089. Epub 2023 Jul 18.
A novel manganese-nitrogen co-doped biochar (MnN@BC) was synthesized and used as particle electrodes in three-dimensional (3D) electro-activation of peroxydisulfate (PDS) for the degradation of refractory organic pollutants. All the spectroscopy (EDS, XRD, XPS, FTIR, and Raman) results indicated that Mn-N nanoclusters were successfully deposited and embedded in BC. The material appeared graphitized structure with more defects after Mn-N doping. MnN@BC in 3D electro-activation of PDS (E/MnN@BC/PDS) exhibited excellent performance in carbamazepine (CBZ) removal, with removal efficiency and degradation rates of 96.84% and 0.0582 min, respectively. Besides, MnN@BC was favorable for adsorption, electron transfer, and reactive oxidizing species (ROS) formation. MnN@BC had good recyclability in the E/MnN@BC/PDS system by the recycled experiments and characterization. Furthermore, quenching experiments, probe experiments, and electron paramagnetic resonance (EPR) analyses suggested that •OH and O were the main ROS in the E/MnN@BC/PDS system, and the non-radical oxidation take a key part. In addition, this system achieved excellent CBZ degradation under wide pH range of 3-11, had good tolerance to natural organic matter and inorganic ions, and was efficient to various water matrices and other refractory organic pollutants. These findings provided new insights into particle electrode design and mechanisms enhancement in electro-activated PDS systems.
合成了一种新型的锰氮共掺杂生物炭（MnN@BC），并将其用作过二硫酸盐（PDS）三维（3D）电活化降解难降解有机污染物的颗粒电极。所有光谱（EDS、XRD、XPS、FTIR和拉曼）结果表明，Mn-N纳米团簇成功沉积并嵌入到生物炭中。Mn-N掺杂后，材料呈现出具有更多缺陷的石墨化结构。MnN@BC在PDS的3D电活化（E/MnN@BC/PDS）中对卡马西平（CBZ）的去除表现出优异的性能，去除效率和降解速率分别为96.84%和0.0582 min⁻¹。此外，MnN@BC有利于吸附、电子转移和活性氧化物种（ROS）的形成。通过循环实验和表征，MnN@BC在E/MnN@BC/PDS系统中具有良好的可循环性。此外，猝灭实验、探针实验和电子顺磁共振（EPR）分析表明，•OH和¹O₂是E/MnN@BC/PDS系统中的主要ROS，非自由基氧化起关键作用。此外，该系统在3-11的宽pH范围内实现了优异的CBZ降解，对天然有机物和无机离子具有良好的耐受性，对各种水基质和其他难降解有机污染物均有效。这些发现为电活化PDS系统中的颗粒电极设计和机理增强提供了新的见解。
