在氯化物条件下类电 Fenton 污染物降解中通过电生 HOCl/H2O2 的协同激活提高羟基自由基产量,Environmental Science & Technology

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在氯化物条件下类电 Fenton 污染物降解中通过电生 HOCl/H2O2 的协同激活提高羟基自由基产量
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2023-02-02 , DOI: 10.1021/acs.est.2c07752
Muhammad Rizwan Haider _{1,

2} , Wen-Li Jiang _{1,

3} , Jing-Long Han ₁ , Ayyaz Mahmood ₄ , Ridha Djellabi ₅ , Huiling Liu ₆ , Muhammad Bilal Asif ₇ , Ai-Jie Wang _{1,

2}

Affiliation

通过催化活化次氯酸产生羟基自由基是一种新型的类芬顿过程。然而，在高氯化物条件下形成金属-氯络合物可能会使催化剂失活并降低工艺效率。在此，首次通过无金属、B/N共掺杂碳纳米纤维阴极将原位电生成的HOCl活化为^{· OH，以在高氯条件下降解污染物。}结果显示，在硫酸盐条件下，罗丹明 B (RhB) 在 120 分钟 ( k = 0.036 min ^–1 ) 内降解了 98%，而在氯化物条件下，仅 30 分钟就完全降解 ( k = 0.188 min ^{–1 )。}增强的降解机制包括吸附和穿梭过程，其中吸附将污染物集中在阴极表面，随后它们被阴极处的 HOCl 和 H ₂ O ₂活化产生的大量^• OH 氧化。_{密度泛函理论计算验证了吡啶N作为HOCl和H 2} O ₂活化的活性位点。还通过处理四环素和双酚A以及农药生产厂的高氯真实二级废水来评估工艺效率。^• OH 和 HOCl的高产率允许阴极连续再生几个周期，限制其快速失活，这在实际应用中很有前景。

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Boosting Hydroxyl Radical Yield via Synergistic Activation of Electrogenerated HOCl/H2O2 in Electro-Fenton-like Degradation of Contaminants under Chloride Conditions

Hydroxyl radical production via catalytic activation of HOCl is a new type of Fenton-like process. However, metal–chlorocomplex formation under high chloride conditions could deactivate the catalyst and reduce the process efficiency. Herein, in situ electrogenerated HOCl was activated to ^•OH via a metal-free, B/N-codoped carbon nanofiber cathode for the first time to degrade contaminant under high chloride condition. The results show 98% degradation of rhodamine B (RhB) within 120 min (k = 0.036 min^–1) under sulfate conditions, while complete degradation (k = 0.188 min^–1) was obtained in only 30 min under chloride conditions. An enhanced degradation mechanism consists of an Adsorb & Shuttle process, wherein adsorption concentrates the pollutants at the cathode surface and they are subsequently oxidized by the large amount of ^•OH produced via activation of HOCl and H₂O₂ at the cathode. Density functional theory calculations verify the pyridinic N as the active site for the activation of HOCl and H₂O₂. The process efficiency was also evaluated by treating tetracycline and bisphenol A as well as high chloride-containing real secondary effluents from a pesticide manufacturing plant. High yields of ^•OH and HOCl allow continuous regeneration of the cathode for several cycles, limiting its fast deactivation, which is promising for real application.

更新日期：2023-02-02

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