An observed "sandwich" framework mediated via sulfate ions as electron shuttle for efficient electro-oxidation of organic pollutants

IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Water Research Pub Date : 2025-04-15 Epub Date: 2025-01-13 DOI:10.1016/j.watres.2025.123139
Yucheng Liu, Hongtao Liu, Chen Wang, Haoran Sun, Lizhang Wang
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Abstract

“Electro-oxidation processes are effective in treating sulfate-rich organic wastewater. However, this technology development has been hindered by the poor understanding of the role of sulfate ions. This paper reports that high concentration of sulfate ions significantly enhanced the electro-oxidation of organic pollutants. High sulfate concentration did not affect radical activity or organic pollutant coverage on the electrode surface. We propose that the electrode interface forms a “sandwich” framework mediated by sulfate ions, consisting of the electrode surface, the sulfate ion layer, and the organic pollutant layer. High concentrations of sulfate ions selectively promote the protonated organic pollutant into the framework via electrostatic attraction when the solution pH is lower than the pKa of the organic pollutants. In this framework, the sulfate ion layer acts as an electron shuttle, creating a smooth electron transfer pathway between the electrode surface and the organic maters. In this way, the “sandwich” framework can efficiently electro-oxidize organic pollutants. This study offers new insights into the role of sulfate ions in electro-oxidation processes, redefining their role in pollutant degradation, and guiding the design of sulfate-rich wastewater treatment.”

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一个观察到的“三明治”框架,通过硫酸盐离子作为电子穿梭介导有机污染物的有效电氧化
“电氧化工艺在处理富含硫酸盐的有机废水中是有效的。然而,由于对硫酸盐离子的作用认识不足,阻碍了这项技术的发展。本文报道了高浓度硫酸盐离子对有机污染物的电氧化有显著的促进作用。高硫酸盐浓度不影响电极表面的自由基活性和有机污染物的覆盖。我们提出电极界面形成一个由硫酸盐离子介导的“三明治”框架,由电极表面、硫酸盐离子层和有机污染物层组成。当溶液pH低于有机污染物的pKa时,高浓度的硫酸盐离子通过静电吸引选择性地促进质子化有机污染物进入骨架。在该框架中,硫酸盐离子层充当电子穿梭器,在电极表面和有机物质之间创建了平滑的电子传递途径。通过这种方式,“三明治”框架可以有效地电氧化有机污染物。这项研究为硫酸盐离子在电氧化过程中的作用提供了新的见解,重新定义了它们在污染物降解中的作用,并指导了富硫酸盐废水处理的设计。”
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来源期刊
Water Research
Water Research 环境科学-工程:环境
CiteScore
20.80
自引率
9.40%
发文量
1307
审稿时长
38 days
期刊介绍: Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.
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