A Nature-Inspired Metal-Free Electrocatalyst towards Efficient Electron Transfer and Robust Cascade Oxygen Reduction for Wastewater Treatment

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research Pub Date : 2025-04-28 DOI:10.1016/j.watres.2025.123747

Yao Pan, Xudong Yang, Zhe Wang, Yu Han, Junxi Guo, Ran Yin, Shanyuan Niu, Dan Shan, Lili Ding, Jinfeng Wang, Hongqiang Ren

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Abstract

The pressing demand for removing high-risk emerging contaminants from wastewater calls for tailored treatment strategies, for which heterogeneous electrocatalysis induced by cascade oxygen reduction reaction (ORR) holds considerable potential. This process, however, suffers from poor interfacial electron transfer and discounted performance in non-acidic conditions. Inspired by the electron respiration chain of cells, a metal-free, quinone-based catalyst (PBth-BQ) was innovatively designed and synthesized. With excellent redox reversibility over 50 cycles and no risk of metal leaching, it boosted the direct electron transfer by 110% compared to the bare graphite substrate and facilitated cascade ORR to generate ·OH for effective contaminant abatement in the pH range of 3-13. Among them, pH 8 demonstrated the best performance, which is suitable for wastewater treatment. In particular, PBth-BQ performed well as both anodic and cathodic electrodes in azithromycin mineralization with different oxygen donors, verified by the in-situ mass spectrum. Considering the abundance of quinone-like structures in oxidized carbon materials, this biomimetic design may inspire the further exploration of cheap and efficient electrocatalysts for wastewater treatment.

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一种自然启发的无金属电催化剂用于废水处理的高效电子转移和稳健级联氧还原

从废水中去除高风险新兴污染物的迫切需求需要量身定制的处理策略，其中由级联氧还原反应（ORR）诱导的多相电催化具有相当大的潜力。然而，该工艺在非酸性条件下存在界面电子转移差和性能下降的问题。受细胞电子呼吸链的启发，创新地设计和合成了一种无金属醌基催化剂（PBth-BQ）。在50次循环中具有优异的氧化还原可逆性，没有金属浸出的风险，与裸石墨衬底相比，直接电子转移提高了110%，并促进了级联ORR生成·OH，在pH 3-13范围内有效地减少了污染物。其中pH 8表现出最好的性能，适用于废水处理。通过原位质谱验证，PBth-BQ在不同供氧条件下均表现出良好的阳极和阴极作用。考虑到氧化碳材料中醌类结构的丰富，这种仿生设计可能会激发人们进一步探索廉价高效的废水处理电催化剂。

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来源期刊

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.