Phytic acid pre-modulated and Fe/N co-doped biochar derived from ramie fiber to active persulfate for efficient degradation of tetracycline via radical and non-radical pathways

•Ramie fiber was chosen as the carbon substrate for biochar production.•PA modified ramie fiber biochar provide loading sites for Fe and N.•TCH was eliminated by radical and non-radical pathways in the Fe/N-PABC/PDS system.•Fe/N-PABC/PDS* mediate TCH degradation through electron transfer.•DFT calcul...

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Published inSeparation and purification technology Vol. 342; p. 126976
Main Authors Deng, Yuwei, Xiao, Lixi, Zhou, Huo, Cui, Boyan, Zhang, Lexin, Chen, Dongxinyu, Gu, Chenghui, Zhan, Ziyi, Wang, Rongling, Mei, Shou, Pei, Xuanyuan, Li, Qiang, Ye, Yuxuan, Pan, Fei
Format Journal Article
LanguageEnglish
Published Elsevier B.V 21.08.2024
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Abstract •Ramie fiber was chosen as the carbon substrate for biochar production.•PA modified ramie fiber biochar provide loading sites for Fe and N.•TCH was eliminated by radical and non-radical pathways in the Fe/N-PABC/PDS system.•Fe/N-PABC/PDS* mediate TCH degradation through electron transfer.•DFT calculations reveal synergies among PABC, Fe, and N in TCH degradation. Biochar-driven advanced oxidation processes (AOPs) have been widely applied in water decontamination from recalcitrant organic pollutants, yet its performance is restricted due to the complex functional groups of precursors and the obstacles of regulating the active sites. Herein, we prepared a phytic acid (PA) pre-modulated and Fe/N co-doped biochar derived from ramie fiber (Fe/N-PABC) to activate peroxydisulfate (PDS) for tetracycline hydrochloride (TCH) removal. The pre-treatment by PA facilitates the formation of pore structure and provide abundant loading sites for subsequent iron and nitrogen (Fe, N) doping. The main forms of Fe, N present in Fe/N-PABC are Fe0, Fe (II), pyridine N, and graphite N, respectively. In the presence of Fe/N-PABC, 80 % of TCH were degraded by PDS in 20 min at pH 5.0, whereas only 16.3 % of TCH was removed by single PDS. The oxidation of TCH was affected in the presence of Cl-, NO3–, SO42-, H2PO4- and HCO3–. Meanwhile, the performance was also validated in authentic waters in terms of degradation efficiency of TCH. The synergistic effects of radical and 1O2 dominated non-radical pathways were confirmed with the introduction of Fe, N in the system. Electrochemical oxidation experiments and density functional theory (DFT) calculations unveiled the electron transfer pathway and the key role of Fe/N-PABC/PDS* as an intermediate oxide. The possible degradation pathways were proposed based on the identification of degradation products. This study sheds light on the innovative concepts for modulating functional biochar and offering fundamental mechanisms of antibiotic degradation in wastewater treatment.
AbstractList •Ramie fiber was chosen as the carbon substrate for biochar production.•PA modified ramie fiber biochar provide loading sites for Fe and N.•TCH was eliminated by radical and non-radical pathways in the Fe/N-PABC/PDS system.•Fe/N-PABC/PDS* mediate TCH degradation through electron transfer.•DFT calculations reveal synergies among PABC, Fe, and N in TCH degradation. Biochar-driven advanced oxidation processes (AOPs) have been widely applied in water decontamination from recalcitrant organic pollutants, yet its performance is restricted due to the complex functional groups of precursors and the obstacles of regulating the active sites. Herein, we prepared a phytic acid (PA) pre-modulated and Fe/N co-doped biochar derived from ramie fiber (Fe/N-PABC) to activate peroxydisulfate (PDS) for tetracycline hydrochloride (TCH) removal. The pre-treatment by PA facilitates the formation of pore structure and provide abundant loading sites for subsequent iron and nitrogen (Fe, N) doping. The main forms of Fe, N present in Fe/N-PABC are Fe0, Fe (II), pyridine N, and graphite N, respectively. In the presence of Fe/N-PABC, 80 % of TCH were degraded by PDS in 20 min at pH 5.0, whereas only 16.3 % of TCH was removed by single PDS. The oxidation of TCH was affected in the presence of Cl-, NO3–, SO42-, H2PO4- and HCO3–. Meanwhile, the performance was also validated in authentic waters in terms of degradation efficiency of TCH. The synergistic effects of radical and 1O2 dominated non-radical pathways were confirmed with the introduction of Fe, N in the system. Electrochemical oxidation experiments and density functional theory (DFT) calculations unveiled the electron transfer pathway and the key role of Fe/N-PABC/PDS* as an intermediate oxide. The possible degradation pathways were proposed based on the identification of degradation products. This study sheds light on the innovative concepts for modulating functional biochar and offering fundamental mechanisms of antibiotic degradation in wastewater treatment.
ArticleNumber 126976
Author Gu, Chenghui
Chen, Dongxinyu
Zhou, Huo
Pei, Xuanyuan
Ye, Yuxuan
Zhan, Ziyi
Cui, Boyan
Wang, Rongling
Li, Qiang
Pan, Fei
Xiao, Lixi
Deng, Yuwei
Zhang, Lexin
Mei, Shou
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Keywords Peroxydisulfate
Fe/N co-doping
Biochar
Phytic acid
Tetracycline
Language English
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Snippet •Ramie fiber was chosen as the carbon substrate for biochar production.•PA modified ramie fiber biochar provide loading sites for Fe and N.•TCH was eliminated...
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SourceType Enrichment Source
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StartPage 126976
SubjectTerms Biochar
Fe/N co-doping
Peroxydisulfate
Phytic acid
Tetracycline
Title Phytic acid pre-modulated and Fe/N co-doped biochar derived from ramie fiber to active persulfate for efficient degradation of tetracycline via radical and non-radical pathways
URI https://dx.doi.org/10.1016/j.seppur.2024.126976
Volume 342
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