Revealing the mechanism of boron doping concentration of boron-doped diamond film electrode on the electrochemical oxidative degradation of perfluorooctanoic acid

IF 4.3 3区材料科学 Q2 MATERIALS SCIENCE, COATINGS & FILMS

Diamond and Related Materials Pub Date : 2025-06-12 DOI:10.1016/j.diamond.2025.112548

Chengcheng Lv , Chuyan Zhang , Bin Chen , Zhaofeng Zhai , Junyao Li , Yvkun Yan , Tianwen Hu , Haozhe Song , Yvhua Yang , Lusheng Liu , Guihong Song , Nan Huang

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引用次数: 0

Abstract

Perfluorooctanoic acid (PFOA) is a great threat to personal safety due to its high bond energy and great electronegativity hard to remove and toxicity. The degradation of PFOA by electrochemical oxidation (EO) using boron-doped diamond (BDD) film electrodes is one of the promising technologies in terms of the efficient, environmentally friendly and controllable. In this study, three BDD film electrodes (BDD₂₀, BDD₃₀, and BDD₄₀) with different boron-doped concentrations were used to degrade PFOA by EO. The results show that BDD₄₀ is the most effective in the removal of both PFOA and total organic carbon (TOC) (∼100 % of PFOA and 92.71 % of TOC were removed after 3 h). The concentration of ·OH was examined by electron paramagnetic resonance (EPR), and it was found that the highest ·OH were produced in BDD₄₀, with a concentration of 4.468 × 10¹¹ spins/mm³ at 40 min. Through the quenching experiment, the roles of

{SO}_{4}^{• -}

and ·OH have been investigated, respectively. Namely,

{SO}_{4}^{• -}

is involved in decarboxylation, while ·OH is used for defluorination. The results and discussion will contribute to a better understanding of the degradation mechanism of PFOA and expand the application of BDD film electrodes in EO, which will ultimately mitigate the risk of PFOA to the environment and health.

Abstract Image

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揭示掺硼金刚石膜电极硼掺杂浓度对全氟辛酸电化学氧化降解的机理

全氟辛酸（PFOA）化学键能高，电负性大，难以去除，毒性大，对人身安全构成极大威胁。利用掺硼金刚石（BDD）膜电极电化学氧化（EO）降解PFOA是一种高效、环保、可控的极具发展前景的技术。本研究采用三种不同掺硼浓度的BDD薄膜电极（BDD20、BDD30和BDD40）对PFOA进行EO降解。结果表明，BDD40对PFOA和总有机碳（TOC）的去除率最高（3 h后PFOA去除率为100%，TOC去除率为92.71%）。通过电子顺磁共振（EPR）检测了·OH的浓度，发现BDD40在40 min时产生的·OH浓度最高，为4.468 × 1011自旋/mm3。通过淬火实验，分别考察了SO4•-和·OH的作用。即SO4•-参与脱羧，而·OH参与脱氟。研究结果将有助于进一步了解PFOA的降解机理，扩大BDD膜电极在EO中的应用，最终减轻PFOA对环境和健康的危害。

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来源期刊

Diamond and Related Materials 工程技术-材料科学：综合

CiteScore

6.00

自引率

14.60%

发文量

702

审稿时长

2.1 months

期刊介绍： DRM is a leading international journal that publishes new fundamental and applied research on all forms of diamond, the integration of diamond with other advanced materials and development of technologies exploiting diamond. The synthesis, characterization and processing of single crystal diamond, polycrystalline films, nanodiamond powders and heterostructures with other advanced materials are encouraged topics for technical and review articles. In addition to diamond, the journal publishes manuscripts on the synthesis, characterization and application of other related materials including diamond-like carbons, carbon nanotubes, graphene, and boron and carbon nitrides. Articles are sought on the chemical functionalization of diamond and related materials as well as their use in electrochemistry, energy storage and conversion, chemical and biological sensing, imaging, thermal management, photonic and quantum applications, electron emission and electronic devices. The International Conference on Diamond and Carbon Materials has evolved into the largest and most well attended forum in the field of diamond, providing a forum to showcase the latest results in the science and technology of diamond and other carbon materials such as carbon nanotubes, graphene, and diamond-like carbon. Run annually in association with Diamond and Related Materials the conference provides junior and established researchers the opportunity to exchange the latest results ranging from fundamental physical and chemical concepts to applied research focusing on the next generation carbon-based devices.