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 in | Separation and purification technology Vol. 342; p. 126976 |
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Main Authors | , , , , , , , , , , , , , |
Format | Journal Article |
Language | English |
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. |
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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 |
Author_xml | – sequence: 1 givenname: Yuwei surname: Deng fullname: Deng, Yuwei organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 2 givenname: Lixi surname: Xiao fullname: Xiao, Lixi organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 3 givenname: Huo surname: Zhou fullname: Zhou, Huo organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 4 givenname: Boyan surname: Cui fullname: Cui, Boyan organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 5 givenname: Lexin surname: Zhang fullname: Zhang, Lexin organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 6 givenname: Dongxinyu surname: Chen fullname: Chen, Dongxinyu organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 7 givenname: Chenghui surname: Gu fullname: Gu, Chenghui organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 8 givenname: Ziyi surname: Zhan fullname: Zhan, Ziyi organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 9 givenname: Rongling surname: Wang fullname: Wang, Rongling organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 10 givenname: Shou surname: Mei fullname: Mei, Shou organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 11 givenname: Xuanyuan surname: Pei fullname: Pei, Xuanyuan organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 12 givenname: Qiang surname: Li fullname: Li, Qiang organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 13 givenname: Yuxuan surname: Ye fullname: Ye, Yuxuan email: yxye@wtu.edu.cn organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China – sequence: 14 givenname: Fei orcidid: 0000-0002-1106-3766 surname: Pan fullname: Pan, Fei email: fpan@wtu.edu.cn organization: School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China |
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Keywords | Peroxydisulfate Fe/N co-doping Biochar Phytic acid Tetracycline |
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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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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 |
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