Journal
CHEMICAL ENGINEERING JOURNAL
Volume 434, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.134732
Keywords
Persulfate activation; Tetracycline; Degradation pathway; Products toxicity; Heteroatoms co-doped g-C3N4
Categories
Funding
- National Natural Science Foundation of China [51808215, 41877491]
- Innovation platform and talent plan of Hunan Province [2020RC2056]
- Provincial Natural Science Foundation of Hunan [2019JJ50253]
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In this study, a porous thin layered Fe, Co and O co-doped g-C3N4 material (FCOCN) was synthesized and used for tetracycline (TC) degradation. The results showed that FCOCN had higher degradation efficiency and kinetic constant in the presence of persulfate (PS). The efficiency of the reaction was improved by modulating the electronic structure and specific surface area of the material. FCOCN also exhibited good degradation performance for organic compounds in water and showed high TC elimination in various matrices.
In this work, the porously thin layered Fe, Co and O co -doped g -C3N4 (FCOCN) was synthesized as persulfate (PS) activator for tetracycline (TC) degradation. The characterization demonstrated that Fe, Co and O doping could boost the specific surface area and modulate the electronic structure of g -C3N4. With addition of PS, the FCOCN2 exhibited the maximum TC removal efficiency of 90.1 % after 120 min reaction, and the kinetic constant was 2.67 times that of pure g-C3N4. Meanwhile, the removal ratio of total organic carbon and reaction stoichiometric efficiency of PS could reach to 68.6% and 5.2%, respectively. When the addition of catalyst and PS were 0.6 g/L and 10.5 mM, respectively, the lower pH and TC concentration, as well as higher temperature were conducive to degradation reaction with activation energy at 23.88 kJ.mol(-1). As indicated by work function, a lower internal electronic excitation energy barrier enhanced electron transfer, so the active species of & BULL;O-2(-), O-1(2), SO4 & BULL;-, SO5 (& BULL;-) and & BULL;OH could be favorably generated on over metal (II/III) redox shuttles, electron -rich O/N and electron-deficient C active sites. The quantitative structure -toxicity relationship prediction of intermediates and the acute toxicity experiment showed that the toxicity of water treated for 60 min to V. fischeri, E. coli and B. subtilis was significantly reduced. Moreover, after five consecutive degradation cycles, the removal efficiency of TC still remained at 72.7%. Besides, even in matrices of tap water, river water, municipal wastewater and medical wastewater, the elimination proportion of TC by FCOCN2/PS were 90.0%, 88.6%, 74.0% and 81.5%, respectively. Hence, the FCOCN2/PS system may be a promising alternative for highly effective treatment of antibiotic contained wastewater and environmental protection.
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