☆ 4.7 Article

N-doped low-rank coal based carbon catalysts for heterogeneous activation of peroxymonosulfate for ofloxacin oxidation via electron transfer and non-radical pathway

JOURNAL OF THE TAIWAN INSTITUTE OF CHEMICAL ENGINEERS (2022)

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JOURNAL OF THE TAIWAN INSTITUTE OF CHEMICAL ENGINEERS

卷 135, 期 -, 页码 -

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DOI: 10.1016/j.jtice.2022.104352

关键词

N-doped carbon catalysts; Peroxymonosulfate; O floxacin(OFL); Non-radicals; Electron transfer

类别

Engineering, Chemical

资金

National Natural Science Foundation of China [52074176, 51904174]
Natural Science Foundation of Shandong Province [ZR2020ME106, ZR2019BEE075]
Natural Science Foundation of Shandong Province Youth Project [ZR2021QE067, ZR2021QE208]
Young Science and Technology Innovation Program of Shandong Province [2020KJD001]
National College Student Innovationand Entrepreneurship Training Program [202110424171]

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In this study, N-doped low-rank coal based carbon catalysts (NLCs) with high graphitization and electrical conductivity were prepared and showed excellent catalytic performance for peroxymonosulfate (PMS) activation. Mechanistic studies revealed that singlet oxygen (1O2) was the main reactive oxygen species in the NLC/PMS system, and electron transfer pathways and surface-bound reactive complexes played an important role. The NLC/PMS system had a wide pH adaptation and good environment adaptation, and could remove pollutants in a pH range of 3-9. Therefore, the prepared N-doped coal based carbon catalytic materials had great prospects for application in advanced oxidation processes for wastewater treatment.

Background: Advanced oxidation processes based on sulfate radicals were promising technologies for deep wastewater treatment. There was an urgent need of low-cost and green catalytic materials. Methods: In this study, N-doped low-rank coal based carbon catalysts (NLCs) were prepared under different urea and low-order coal ratios and pyrolysis temperatures, which showed excellent catalytic performance for peroxymonosulfate (PMS) activation. Significant findings: The NLCs had a high degree of graphitization and electrical conductivity, which leading to a high removal rates as 100% in 45 min. The N-doped structure lead to the formation of electron-rich regions, which favored the adsorption of PMS. Mechanistic studies revealed that the main reactive oxygen species in the NLC/PMS system was singlet oxygen (1O2), and that electron transfer pathways and surface-bound reactive complexes also played an important role in this system. The NLC/PMS system had a wide pH adaptation and good environment adaptation because of the electron transfer mechanism. It could remove 100% OFL in the pH range of 3-9. Therefore, the prepared N-doped coal based carbon catalytic materials had good prospects for application in advanced oxidation processes for wastewater treatment. (c) 2022 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

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Insight into the difference in activation of peroxymonosulfate with nitrogen-doped and non-doped carbon catalysts to degrade bisphenol A

Chen Chen, Caiyun Jiang, Wang Cao, Haifei Zhou, Yuping Wang

Summary: Heteroatom-modified carbon-based catalysts, particularly nitrogen-doped ones, are effective in activating peroxymonosulfate. However, the study found that graphitized carbon nanomaterial GC800 exhibited similar catalytic capacity as nitrogen-doped NGC800 in degrading BPA, but with a higher degradation rate constant. The surface chemistry of carbon materials plays a significant role in catalytic velocity, with GC800 showing a multi-pathway synergy dominated by non-radical electron transfer.

JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING (2021)