Correlation between biochar pore structure-nitrogen defects and tetracycline hydrochloride degradation
WANG Qing, NI Jing-xuan, GAO Yuan
Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China
Abstract：Different pore structure and nitrogen defects of biochar materials were prepared in this work. The dynamic data of adsorption and persulfate-based advanced oxidation process (catalysis) systems were combined with the nitrogen adsorption -desorption test, X-ray photoelectron spectroscopy, Raman test and other characterization methods. They were used to analysis the correlation of pore structure-nitrogen defects and typical antibiotics (tetracycline hydrochloride) degradation systematically and deeply. The results showed that mesoporous surface area and specific surface area were most correlated with persulfate reaction. Nitrogen, especially graphite nitrogen (R2=0.9766) and pyridine nitrogen (R2=0.9596), was the most relevant elements to the reaction process of the system. In addition, the correlation between pore structure and the results was basically same in adsorption and catalysis processes. But nitrogen showed greater correlation in catalysis system than adsorption. Through quenching experiment, linear sweep voltammetry and Raman test, it was found that the catalysis was mainly dominated by singlet oxygen, which meant it was nonradical pathway. Finally, a better preparation direction for biochar materials to be used as activators in the persulfate-based advanced oxidation process of tetracycline hydrochloride was provided. Biochar materials with larger mesoporous surface area, larger specific surface area and more nitrogen, especially graphite nitrogen and pyridine nitrogen should be prepared for the catalysis of tetracycline hydrochloride.
Chen G, Yu Y, Liang L, et al. Remediation of antibiotic wastewater by coupled photocatalytic and persulfate oxidation system:A critical review[J]. J Hazard Mater, 2021,408:124461.
[2]
Zhu T T, Su Z X, Lai W X, et al. Insights into the fate and removal of antibiotics and antibiotic resistance genes using biological wastewater treatment technology[J]. Science of The Total Environment, 2021, 776:145906.
[3]
Dai Y, Liu M, Li J, et al. A review on pollution situation and treatment methods of tetracycline in groundwater[J]. Separation Science and Technology, 2019,55(5):1005-1021.
[4]
Wang H, Guo W, Yin R, et al. Biochar-induced Fe (III) reduction for persulfate activation in sulfamethoxazole degradation:Insight into the electron transfer, radical oxidation and degradation pathways[J]. Chemical Engineering Journal, 2019,362:561-569.
[5]
Duan X, Sun H, Shao Z, et al. Nonradical reactions in environmental remediation processes:Uncertainty and challenges[J]. Applied Catalysis B:Environmental, 2018,224:973-982.
[6]
Wang X, Wang A, Ma J. Visible-light-driven photocatalytic removal of antibiotics by newly designed C3N4@MnFe2O4-graphene nanocomposites[J]. Journal of Hazardous Materials, 2017,336:81-92.
[7]
Kakavandi B, Bahari N, Rezaei Kalantary R, et al. Enhanced sonophotocatalysis of tetracycline antibiotic using TiO2decorated on magnetic activated carbon (MAC@T) coupled with US and UV:A new hybrid system[J]. Ultrason Sonochem, 2019,55:75-85.
[8]
Cui C, Jin L, Jiang L, et al. Removal of trace level amounts of twelve sulfonamides from drinking water by UV-activated peroxymonosulfate[J]. Science of the Total Environment, 2016,572:244-251.
[9]
刘佳露,张凤君,彭新晶.非均相活化剂磁性纳米CoFe2O4的制备及其活性评价[J].中国环境科学, 2021,41(5):2179-2186. Liu J L, Zhang F J, Peng X J. Preparation and activity evaluation of heterogeneous magnetic nano-CoFe2O4activators[J]. China Environmental Science, 2021,41(5):2179-2186.
[10]
翟文琰,李孟,张倩.过硫酸盐协同光催化纳米ZnO降解盐酸四环素的影响机制[J].中国环境科学, 2020,40(6):2483-2492. Zhai W Y, Li M, Zhang Q. Influence mechanism and synergistic effects of photocatalytic degradation of tetracycline hydrochloride by the combinationof persulfate and nano-ZnO[J].China Environmental Science, 2020,40(6):2483-2492.
[11]
苏冰琴,刘一清,林昱廷,等.Fe3O4活化过硫酸盐体系同步去除诺氟沙星和铅[J].中国环境科学, 2022,42(2):717-727. Su B Q, Liu Y Q, Lin Y T, et al. Simultaneous removal of norfloxacin and Pb (II) via Fe3O4-activated persulfate oxidation[J]. China Environmental Science, 2022,42(2):717-727.
[12]
Pan J, Gao B, Duan P, et al. Recycling exhausted magnetic biochar with adsorbed Cu2+as a cost-effective permonosulfate activator for norfloxacin degradation:Cu contribution and mechanism[J]. Journal of Hazardous Materials, 2021,413:125413.
[13]
Li Z, Sun Y, Yang Y, et al. Comparing biochar-and bentonitesupported Fe-based catalysts for selective degradation of antibiotics:Mechanisms and pathway[J]. Environmental Research, 2020,183:109156.
[14]
Huo X, Zhou P, Zhang J, et al. N, S-Doped porous carbons for persulfate activation to remove tetracycline:Nonradical mechanism[J]. Journal of Hazardous Materials, 2020,391:122055.
[15]
Yang Z, Li Y, Zhang X, et al. Sludge activated carbon-based CoFe2O4-SAC nanocomposites used as heterogeneous catalysts for degrading antibiotic norfloxacin through activating peroxymonosulfate[J]. Chemical Engineering Journal, 2020,384:123319.
[16]
Wang B, Li Y N, Wang L. Metal-free activation of persulfates by corn stalk biochar for the degradation of antibiotic norfloxacin:Activation factors and degradation mechanism[J]. Chemosphere, 2019,237:124454.
[17]
Ren W, Xiong L, Nie G, et al. Insights into the electron-transfer regime of peroxydisulfate activation on carbon nanotubes:the role of oxygen functional groups[J]. Environmental Science&Technology, 2020,54(2):1267-1275.
[18]
Chen C, Ma T, Shang Y, et al. In-situ pyrolysis of Enteromorpha as carbocatalyst for catalytic removal of organic contaminants:Considering the intrinsic N/Fe in Enteromorpha and non-radical reaction[J]. Catalysis B:Environmental, 2019,250:382-395.
[19]
雷倩,许路,艾伟,等.CDs-BOC复合催化剂可见光下活化过硫酸盐降解典型PPCPs[J].环境科学, 2021,42(6):2885-2895. Lei Q, Xu L, Ai W,et al. CDs-BOC nanophotocatalyst activating persulfate under visible light for the efficient degradation of typical PPCPs[J]. Environmental Science, 2021,42(6):2885-2895.
[20]
Liu L, Xu X, Li Y, et al. One-step synthesis of "nuclear-shell" structure iron-carbon nanocomposite as a persulfate activator for bisphenol A degradation[J]. Chemical Engineering Journal, 2020,382:122780.
[21]
张荣荣,崔育倩,孙媛媛. FeS/碳纤维活化过一硫酸盐高效降解水中四环素[C]//2020中国环境科学学会科学技术年会论文集.北京:中国环境科学出版社, 2020:933-941. Zhang R R, Cui Y Q, Sun Y Y. Efficient degradation of tetracycline in water via a sulfate activated by FeS/Carbon fiber[C]//2020 Proceedings of annual Conference of Chinese Society for Environmental Science. Beijing:China Environmental Science Press, 2020:933-941.
[22]
Kang J, Zhang H, Duan X, et al. Nickel in hierarchically structured nitrogen-doped graphene for robust and promoted degradation of antibiotics[J]. Journal of Cleaner Production, 2019,218:202-211.
[23]
Li X J, Yu X X, Liu J Y, et al. Synthesis of nitrogen-doped graphene via thermal annealing graphene with urea[J]. Chinese Journal of Chemical Physics, 2012,25(3):325-329.
[24]
Yin R, Guo W, Ren N, et al. New insight into the substituents affecting the peroxydisulfate nonradical oxidation of sulfonamides in water[J]. Water Research, 2020,171:115374.
