Manipulating carbon defects for rapid H2O2 and ·OH formation: A strategy for efficient electrocatalytic organic pollutant degradation

IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-09-11 Epub Date: 2025-03-18 DOI:10.1016/j.seppur.2025.132610
Ying Gao , Yang Wang , Yuxin Liu , Haoyu Wang , Guohui Dong
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Abstract

Recently, carbon-based materials (CNMs) have garnered significant interest within the domain of electrocatalytic pollutant remediation. However, the ambiguity surrounding the specific active sites on CNMs hinders the enhancement of their oxidation capabilities. Here, a series of samples were designed to elucidate the actual sites by manipulating the quantity of oxygen-containing functional groups and carbon defects on CNMs (DRG-x). Among the DRG-x, DRG-600 demonstrated superior activity in hydrogen peroxide (H2O2) generation, and exhibited the highest kinetic activity for tetracycline degradation. Interestingly, carbon defects, rather than oxygen − containing functional groups, predominantly boosted the generation of H2O2 and hydroxyl radicals (·OH), thereby endowing it with exceptional pollutant removal efficiency. Besides, through the systematic determinations of reactive oxygen species (H2O2, ·OH and singlet oxygen) within the electrolyte, it was evident that ·OH constitutes 79.3% and plays a pivotal role in the degradation process. This work provided a reference for strategically enhancing the activity of CNMs, particularly in terms of augmenting its electrocatalytic performance and organic degradation capabilities.

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操纵碳缺陷快速形成H2O2和·OH:一种有效的电催化有机污染物降解策略
最近,碳基材料(CNMs)在电催化污染物修复领域引起了极大的兴趣。然而,围绕cnm上特定活性位点的模糊性阻碍了其氧化能力的增强。本文设计了一系列样品,通过控制CNMs (DRG-x)上含氧官能团和碳缺陷的数量来阐明实际的位点。DRG-x中,DRG-600对过氧化氢(H2O2)的生成具有较强的活性,对四环素的降解具有最高的动力学活性。有趣的是,碳缺陷,而不是含氧官能团,主要促进H2O2和羟基自由基(·OH)的产生,从而赋予其特殊的污染物去除效率。此外,通过对电解液中活性氧(H2O2、·OH和单线态氧)的系统测定,发现·OH占79.3%,在降解过程中起关键作用。这项工作为战略性地提高cnm的活性,特别是在提高其电催化性能和有机降解能力方面提供了参考。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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