Enhancing catalytic activity of CuCoFe-layered double oxide towards peroxymonosulfate activation by coupling with biochar derived from durian peel for antibiotic degradation: The role of C=O in biochar and underlying mechanism of built-in electric field
CuCoFe-LDO/BCD was successfully synthesized from CuCoFe-LDH and biochar derived from durian shell (BCD). Ciprofloxacin (CFX) degraded more than 95% mainly by O2•− and 1O2 in CuCoFe-LDO/BCD(2/1)/PMS system within 10 min with a rate constant of 0.255 min−1, which was 14.35 and 2.66 times higher than t...
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Published in | Chemosphere (Oxford) Vol. 361; p. 142452 |
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Main Authors | , , , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
England
Elsevier Ltd
01.08.2024
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Subjects | |
Online Access | Get full text |
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Summary: | CuCoFe-LDO/BCD was successfully synthesized from CuCoFe-LDH and biochar derived from durian shell (BCD). Ciprofloxacin (CFX) degraded more than 95% mainly by O2•− and 1O2 in CuCoFe-LDO/BCD(2/1)/PMS system within 10 min with a rate constant of 0.255 min−1, which was 14.35 and 2.66 times higher than those in BCD/PMS and CuCoFe-LDO/PMS systems, respectively. The catalytic system exhibited good performance over a wide pH range (3–9) and high degradation efficiency of other antibiotics. Built-in electric field (BIEF) driven by large difference in the work function/Fermi level ratio between CuCoFe-LDO and BCD accelerated continuous electron transfer from CuCoFe-LDO to BCD to result in two different microenvironments with opposite charges at the interface, which enhanced PMS adsorption and activation via different directions. As a non-radical, 1O2 was mainly generated via PMS activation by C=O in BCD. The presence of C=O in BCD resulted in an increase in atomic charge of C in C=O and redistributed the charge density of other C atoms. As a result, strong adsorption of PMS at C atom in C=O and other C with a high positive charge was favorable for 1O2 generation, whereas an enhanced adsorption of PMS at negatively charged C accounted for the generation of •OH and SO4•−. After adsorption, electrons in C of BCD became deficient and were fulfilled with those transferred from CuCoFe-LDO driven by BIEF, which ensured the high catalytic activity of CuCoFe-LDO/BCD. O2•−, on the other hand, was generated via several pathways that involved in the transformation of •OH and SO4•− originated from PMS activation by the transition of metal species in CuCoFe-LDO and negatively charged C in BCD. This study proposed a new idea of fabricating a low-cost metal-LDH and biomass-derived catalyst with a strong synergistic effect induced by BIEF for enhancing PMS activation and antibiotic degradation.
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•Durian peel-derived biochar enhances CFX degradation in CuCoFe-LDO/BCD/PMS by 1.48 times.•The role of C=O in BCD for PMS activation and 1O2 generation is confirmed by DFT calculations.•A new pathway for 1O2 generation via PMS activation by C=O is proposed.•Built-in electric field between CuCoFe-LDO and BCD accelerates electron transfer and enhances PMS activation.•CFX degradation is contributed mainly by both radical (O2•−) and non-radical (1O2). |
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Bibliography: | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
ISSN: | 0045-6535 1879-1298 1879-1298 |
DOI: | 10.1016/j.chemosphere.2024.142452 |