4.8 Article

Reactive Nitrogen Species Generated by Gas-Liquid Dielectric Barrier Discharge for Efficient Degradation of Perfluorooctanoic Acid from Water

Journal

ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 56, Issue 1, Pages 349-360

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.est.1c06342

Keywords

gas-liquid mixed discharge; dielectric barrier discharge; perfluorooctanoic acid; oxidative degradation; reactive nitrogen species

Funding

  1. National Natural Science Foundation of China [51979039, 51708096, 21906016]
  2. Fundamental Research Funds for the Central Universities [2232019A3-10, 2232020D-25]
  3. International Cooperative Projects of Shanghai Municipal Committee of Science and Technology [18230722800]

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The novel GLDBD reactor was designed to efficiently degrade PFOA with removal efficiencies over 98.0% within 50 minutes and energy yields exceeding 114.5 mg.kWh(-1). Reactive nitrogen species were identified as crucial for PFOA degradation in the plasma system, making the reactor less sensitive to various water matrices and promising for practical application. The research proposed possible PFOA degradation pathways based on LC-MS results and DFT calculation, providing an effective and versatile alternative for PFOA removal from different water matrices.
Perfluorooctanoic acid (PFOA) poses a serious threat to the ecological environment and biological health because of its ubiquitous distribution, extreme persistence, and high toxicity. In this study, we designed a novel gas-liquid dielectric barrier discharge (GLDBD) reactor which could efficiently destruct PFOA. PFOA removal efficiencies can be obtained in various water matrices, which were higher than 98.0% within 50 min, with energy yields higher than 114.5 mg.kWh(-1). It was confirmed that the reactive species including e(-), ONOOH, center dot NO2, and hydroxyl radicals (center dot OH) were responsible for PFOA removal. Especially, this study first revealed the crucial role of reactive nitrogen species (RNS) for PFOA degradation in the plasma system. Due to the generation of a large amount of RNS, the designed GLDBD reactor proved to be less sensitive to various water matrices, which meant a broader promising practical application. Moreover, influential factors including high concentration of various ions and humic acid (HA), were investigated. The possible PFOA degradation pathways were proposed based on liquid chromatograph-mass spectrometer (LC-MS) results and density functional theory (DFT) calculation, which further confirmed the feasibility of PFOA removal with RNS. This research, therefore, provides an effective and versatile alternative for PFOA removal from various water matrices.

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