Details zur Publikation |
| Kategorie | Textpublikation |
| Referenztyp | Zeitschriften |
| DOI | 10.1016/j.cej.2024.155252 |
Lizenz  |
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| Titel (primär) | In situ anchoring of bimetal (Cu, Fe) sulfides featured by sulfur vacancy and phosphorus doping within porous carbon nanocubes derived from Prussian blue analogs to activate peroxymonosulfate for the efficient degradation of organic pollutants |
| Autor | Chang, J.; Xia, S.; Shi, Z.; Zeng, H.; Zhang, H.
; Deng, L. |
| Quelle | Chemical Engineering Journal |
| Erscheinungsjahr | 2024 |
| Department | TECH |
| Band/Volume | 498 |
| Seite von | art. 155252 |
| Sprache | englisch |
| Topic | T7 Bioeconomy |
| Supplements | Supplement 1 |
| Keywords | Sulfur vacancy; Phosphorus doping; Peroxymonosulfate; Electron-transfer; Sulfadiazine degradation |
| Abstract | In this work, Prussian blue analogues (CuFe-PBA) derived copper-iron sulfides/N-doped porous carbon composite (CuFe-NC-SP-x)
was prepared as an effective peroxymonosulfate (PMS) activator to
degrade sulfadiazine (SDZ). A strategy that kills two birds with one
stone was proposed to construct CuFe-NC-SP-x, i.e., S-etched CuFe-PBA (CuFe-PBA-S) was annealed with NaH2PO2 in N2
atmosphere to simultaneously introduce sulfur vacancy (Sv) and
phosphorus doping. 40 μM SDZ was completely removed by CuFe-NC-SP-2/PMS
in 20 min (0.2 g/L catalyst and 0.5 mM PMS). The kobs value obtained by CuFe-NC-SP-2 (0.48 min−1) was nearly 33 and 17 times higher than that of CuFe-PBA (0.014 min−1) and CuFe-PBA-S (0.028 min−1),
respectively. Quenching tests, electron paramagnetic resonance (EPR)
analysis indicated that PMS activation in the system involved radical
pathway (26.1 %  OH and 22.7 % SO4–) and non-radical pathway (17.8 % 1O2 and 33.4 % electron transfer process). OH, SO4– and 1O2
were mainly produced by S enhanced metal sites for PMS activation. The
synergistic effect of Sv and P doping enabled the powerful electron
transfer mechanism. Electrochemical tests and DFT calculations
demonstrated that Sv existing in CuFe-NC-SP-x improved the
electron donor ability and increased the adsorption energy toward PMS,
and phosphorus doping accelerated the electron transport from SDZ to
PMS. This work not only provides a novel strategy to synthesize a high
effective PMS activator by introducing Sv and phosphorous doing in one
step, but also manages to comprehensively understand the electron
transfer activation mechanisms of PMS facilitated by Sv and phosphorous
doping. |
| dauerhafte UFZ-Verlinkung | https://www.ufz.de/index.php?en=20939&ufzPublicationIdentifier=29708 |
| Chang, J., Xia, S., Shi, Z., Zeng, H., Zhang, H., Deng, L. (2024): In situ anchoring of bimetal (Cu, Fe) sulfides featured by sulfur vacancy and phosphorus doping within porous carbon nanocubes derived from Prussian blue analogs to activate peroxymonosulfate for the efficient degradation of organic pollutants Chem. Eng. J. 498 , art. 155252 10.1016/j.cej.2024.155252 |
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