Revisiting the multipath elimination of contaminants by carbonyl-containing manganese-carbon composites in the peroxymonosulfate system: A new way of constructing C-Mn-PMS complexes to distinguish the stages of active species production

催化作用 降级(电信) 复合数 化学 吸附 碳纤维 密度泛函理论 活动站点 中心组合设计 电子转移 化学工程 材料科学 光化学 复合材料 有机化学 响应面法 计算化学 计算机科学 电信 工程类 色谱法
作者
Huo Zhou,Lixi Xiao,Yangyang Deng,Cheng-Xin Chen,Xuanyuan Pei,Qiang Li,Yuxuan Ye,Fei Pan
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:471: 144685-144685 被引量:9
标识
DOI:10.1016/j.cej.2023.144685
摘要

The use of value-added effects of composite catalysts to enhance the practical application of peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) has been one of the hot topics in the field of environmental remediation. However, the complex structure of the composite catalyst/PMS systems has hindered the exploration of the origin and generation stages of active species. To clarify the relationship between active sites and active species, Mn carbon-based composite/PMS systems with structured active sites were constructed to achieve an effective strategy for organic conversion. This paper investigates the correlation between C = O-Mn and reactive species generation by developing Mn carbon composites with structured active sites (C = O) to activate PMS for the degradation of TCH. Additionally, a pre-oxidation experiment was proposed to divide the whole catalytic degradation process into two stages: oxidation and degradation. The results show that the C = O–Mn–PMS composite intermediate can still effectively degrade Tetracycline after being separated from the solution. The study also revealed the structure–function relationship of different active sites in the C = O-Mn catalyst was revealed by density functional theory (DFT) calculations. The Mn-O, Mn-O-Mn and C = O structures achieved efficient utilization of PMS and rapid degradation of TCH through the adsorption of PMS and single electron transfer generation SO4−, OH, O2−, 1O2. This paper provides new ideas for the reaction mechanism and rational design of catalysts based on the Mn-carbon composite/PMS system.
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