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Peroxymonosulfate activation by iron-carbon composite derived from coal gasification slag for sulfamethoxazole removal: Performance evaluation and mechanism insight

[Display omitted] •Fe-C composite derived from CGS was first prepared for PMS activation.•The catalyst had excellent catalytic ability among the reported metal-C catalysts.•91.1 % of SMX could be degraded within 90 min in the Fe-C composite/PMS system.•Fe species and oxygen-containing functional gro...

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Published in:Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2023-01, Vol.456, p.140996, Article 140996
Main Authors: Long, Yuhan, Yang, Peizhen, Wang, Changyan, Wu, Weiran, Chen, Xi, Liu, Wenhao, Cao, Zhenhua, Zhan, Xuesong, Liu, Dongfang, Huang, Wenli
Format: Article
Language:English
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Summary:[Display omitted] •Fe-C composite derived from CGS was first prepared for PMS activation.•The catalyst had excellent catalytic ability among the reported metal-C catalysts.•91.1 % of SMX could be degraded within 90 min in the Fe-C composite/PMS system.•Fe species and oxygen-containing functional groups contributed to ROS generation.•Surface-bounded radicals, 1O2 and electron transfer removed 87.8% of SMX. A novel iron-carbon (Fe-C) composite was fabricated using coal gasification slag (CGS) as the feedstocks and applied in sulfamethoxazole (SMX) degradation via peroxymonosulfate (PMS) activation. The optimized Fe-C composite (CGS-1000) had excellent catalytic ability among the reported metal-C catalysts, showing a superior SMX degradation capacity (91.1 %) and kinetic reaction rate (0.0177 min−1) within 90 min under the condition of 0.2 g·L−1 CGS-1000, 2.0 mM PMS at ambient pH (6.3). Characterization results illustrated that the relatively larger surface area (102.50 m2·g−1), pore size (3.93 nm), and higher carbon defectiveness (ID/IG = 1.48) of CGS-1000 promoted its SMX degradation performance. XPS and FTIR spectrum revealed that PMS was mainly activated by Fe species and oxygen-containing functional groups (CO, C-OH) on the carbon matrix for the generation of reactive oxygen species (ROS). Notably, surface-bounded radicals (SO4−, OH), singlet oxygen (1O2), and direct electron transfer were primarily involved in the CGS-1000/PMS system, of which the relative contributions to SMX oxidation were calculated to be 25.8 %, 49.5 %, and 12.5 %, respectively. The excellent degradation efficiency should be attributed to the simultaneous SMX oxidation both in solution and on the surface of CGS-1000 through these three oxidation pathways. Finally, four SMX degradation pathways were proposed based on the twelve intermediates detected by LC-MS. The toxicity of the by-products of SMX was alleviated according to the quantitative structure–activity relationship analysis. Overall, these results suggested that CGS-1000 was a high-efficiency PMS catalyst for SMX degradation and provided new insights into the design of other solid waste-derived catalysts.
ISSN:1385-8947
1873-3212
DOI:10.1016/j.cej.2022.140996