An Ning, Zhao Min, Zheng Xiangyong, Wang Qi, Huang Xianfeng, Sun Bo, Shen Yi, Wang Jun, Chen Baoliang, Liu Renlan
College of Life and Environmental Science, Wenzhou University, Wenzhou 325035, China; National and Local Joint Engineering Research Center of Ecological Treatment Technology of Urban Water Pollution, Wenzhou University, Wenzhou 325035, China; Zhejiang Provincial Engineering Laboratory for Ecological Treatment Technology of Urban Water Pollution, Wenzhou University, Wenzhou 325035, China.
College of Environment, Zhejiang University of Technology, Hangzhou 310032, China.
J Hazard Mater. 2022 Feb 15;424(Pt B):127444. doi: 10.1016/j.jhazmat.2021.127444. Epub 2021 Oct 6.
Metal-free carbonaceous catalysts are receiving increasing attention in wastewater treatment. Here, nitrogen and sulfur co-doped carbon sphere catalysts (N,S-CSs-OH) were synthesized using glucose and L-cysteine via a hydrothermal method and high temperature alkali activation. The N,S-CSs-10%-OH exhibited excellent catalytic performance for the degradation of oxytetracycline (OTC). The degradation rate was 95.9% in 60 min, and the reaction equilibrium rate constant was 0.0735 min (k). The synergistic effect of adsorption-promoting degradation was demonstrated in the removal process of OTC. The excellent adsorption capacity of N,S-CSs-10%-OH ensured the efficient oxidation of OTC. N,S-CSs-10%-OH reduced the activation energy of the OTC degradation reaction (Ea=18.23 kJ/mol). Moreover, the pyrrolic N, thiophene S and carbon skeleton played an important role in the degradation of OTC based on density function theory, and the catalytic mechanism was expounded through radical and nonradical pathways. The active species involved in the reaction were O, O, SO and •OH, of which O was the primary reactive species. This study provides a new insight into the reaction mechanism for efficient treatment of organic pollutants using metal-free doped porous carbon materials.
无金属碳质催化剂在废水处理中受到越来越多的关注。在此，通过水热法和高温碱活化，使用葡萄糖和L-半胱氨酸合成了氮硫共掺杂碳球催化剂（N,S-CSs-OH）。N,S-CSs-10%-OH对土霉素（OTC）的降解表现出优异的催化性能。60分钟内降解率为95.9%，反应平衡速率常数为0.0735 min⁻¹（k）。在OTC的去除过程中证明了吸附促进降解的协同作用。N,S-CSs-10%-OH优异的吸附能力确保了OTC的高效氧化。N,S-CSs-10%-OH降低了OTC降解反应的活化能（Ea = 18.23 kJ/mol）。此外，基于密度泛函理论，吡咯氮、噻吩硫和碳骨架在OTC的降解中起重要作用，并通过自由基和非自由基途径阐述了催化机理。参与反应的活性物种为O₂、¹O₂、SO₄²⁻和•OH，其中¹O₂是主要的反应物种。本研究为使用无金属掺杂多孔碳材料高效处理有机污染物的反应机理提供了新的见解。
