Low-coordinated Co-N3 sites induce peroxymonosulfate activation for norfloxacin degradation via high-valent cobalt-oxo species and electron transfer
學年 111
學期 2
出版（發表）日期 2023-05-11
作品名稱 Low-coordinated Co-N3 sites induce peroxymonosulfate activation for norfloxacin degradation via high-valent cobalt-oxo species and electron transfer
作品名稱（其他語言）
著者 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
單位
出版者
著錄名稱、卷期、頁數 Journal of Hazardous Materials 2023, 455, 131622
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.
關鍵字
語言 en
ISSN 0304-3894; 1873-3336
期刊性質 國外
收錄於 SCI
產學合作
通訊作者
審稿制度 否
國別 NLD
公開徵稿
出版型式 ,電子版
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