The effect of N-doping on the synergy between adsorption and 2e-ORR performance of activated carbon cathode in an electro-Fenton system

吸附 阴极 降级(电信) 选择性 兴奋剂 碳纤维 化学 化学工程 活性炭 无机化学 材料科学 催化作用 有机化学 复合数 计算机科学 物理化学 复合材料 工程类 电信 光电子学
作者
Haiqian Zhao,Shuaishuai Han,Jiuyang Jia,Mingqi He,Kaibo An,Ziyu Tang,Shiwei Lai,Xue Yang,Zhonghua Wang
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:468: 143505-143505 被引量:29
标识
DOI:10.1016/j.cej.2023.143505
摘要

The adsorption of carbon materials and 2e-ORR performance can be promoted by N-doping. However, the effect of different N-doping types on adsorption and 2e-ORR and their synergy is not clear, which limits the development of an electro-Fenton system. To enhance the degradation efficiency of the electro-Fenton system, it is essential to understand the mechanisms involved in regulating cathode performance. To achieve this goal, a multi-scale simulation approach was employed that integrates molecular dynamics and quantum chemical simulations. This method was utilized to fabricate carbon planes with various N-doping types. The simulation results showed pyridinic-N and pyrrolic-N showed a cooperative effect and promoted the capacity of activated carbon to adsorb tetracycline. Graphitic-N and pyridinic-N greatly improved the selectivity of 2e-ORR, which is conducive to the formation of H2O2. Experimental investigations have revealed a synergistic association between adsorption and 2e-ORR, and suboptimal performance of either process can hinder the degradation efficacy of electro-Fenton. The reason for this is that an exceptional selectivity of 2e-ORR enhances the production of ·OH, and good adsorption capability facilitates the utilization of ·OH. The MAC cathode exhibits a greater synergistic effect between adsorption and 2e-ORR owing to the suitable proportion of pyridinic-N, pyrrolic-N, and graphitic-N. Under the action of high-efficiency synergy, the degradation effect of tetracycline by the electro-Fenton cathode was 8.72%-11.64% higher than that of other modified cathodes. The outcomes of our investigation provided insights into the approach for targeted control of the performance of N-doped modified cathodes in the electro-Fenton system.
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