Low-coordinated Co-N3 sites induce peroxymonosulfate activation for norfloxacin degradation via high-valent cobalt-oxo species and electron transfer

doi:10.1016/j.jhazmat.2023.131622

淡江大學機構典藏 > 工學院 > 電機工程學系暨研究所 > 期刊論文 > Item 987654321/125745

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題名:	Low-coordinated Co-N3 sites induce peroxymonosulfate activation for norfloxacin degradation via high-valent cobalt-oxo species and electron transfer
作者:	C. Wang, X. Wang, H. Wang, L. Zhang, Y. Wang, C. L. Dong, Y. C. Huang, P. Guo, R. Cai, S. J. Haigh, X. Yang, Y. Sun, and D. Yang
日期:	2023-08-05
上傳時間:	2024-07-31 12:11:33 (UTC+8)
出版者:	Elsevier
摘要:	The identification of reactive species in peroxymonosulfate (PMS) activation triggered by carbon-based single atom catalysts is the key to reveal the pollutant degradation mechanism. Herein, carbon-based single atom catalyst with low-coordinated Co-N3 sites (CoSA-N3-C) was synthesized to active PMS for norfloxacin (NOR) degradation. The CoSA-N3-C/PMS system exhibited consistent high performance for oxidizing NOR over a wide pH range (3.0–11.0). The system also achieved complete NOR degradation in different water matrixes, high cycle stability and excellent degradation performance for other pollutants. Theoretical calculations confirmed that the catalytic activity was derived from the favorable electron density of low-coordinated Co-N3 configuration, which was more conductive to PMS activation than other configurations. Electron paramagnetic resonance spectra, in-situ Raman analysis, solvent exchange (H2O to D2O), salt bridge and quenching experiments concluded that high-valent cobalt(IV)-oxo species (56.75%) and electron transfer (41.22%) contributed dominantly to NOR degradation. Moreover, 1O2 was generated in the activation process while not involved in pollutant degradation. This research demonstrates the specific contributions of nonradicals in PMS activation over Co-N3 sites for pollutant degradation. It also offers updated perceptions for rational design of carbon-based single atom catalysts with appropriate coordination structure.
關聯:	Journal of Hazardous Materials 455, 131622
DOI:	10.1016/j.jhazmat.2023.131622
顯示於類別:	[電機工程學系暨研究所] 期刊論文

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