生物炭活化两种过硫酸盐降解四环素比较分析

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Abstract Corn straw biochar (Y-BC) was prepared by high-temperature pyrolysis method and its structure and morphology properties were characterized with a series of analytical techniques. The effects of initial pH and co-existing ions on tetracycline (TC) removal by Y-BC activated two types of persulfates: peroxydisulfate (PDS) and peroxymonosulfate (PMS) were systematically compared. The results showed that Y-BC activated PDS system could effectively remove TC under acidic and neutral conditions (pH=3~7), and TC removal efficiency was between 69.0% to 75.7% in 60min, while alkaline conditions (pH=9~11) TC removal efficiency reduced to 47.8%~48.4%. In contrast, the Y-BC-activated PMS system demonstrated a broad pH range for TC removal, and TC removal efficiency stabilized at 80.9%~86.8% at initial pH 3~11. The Cl^- and NO₃^- anions exhibited negligible effects on both activated persulfate systems. Meanwhile, HCO₃^- showed an inhibitory effect on TC removal by the Y-BC-activated PDS system while promoting the effect by the Y-BC-activated PMS system. TC removal efficiency decreased by 7.6% and increased by 5.1% with Y-BC-activated PDS and PMS, respectively. Combined the results of X-ray photoelectron spectroscopy, quenching experiments, and electron paramagnetic resonance analysis, it was deduced that the primary active sites for Y-BC activated PDS system were defect structures, and TC degradation was mainly through singlet oxygen (¹O₂) generation and electron transfer mechanisms. Conversely, functional groups served as key active sites for the Y-BC-activated PMS system, and TC degradation was primarily via hydroxyl radical (·OH) formation.

Key words： biochar persulfate tetracycline influencing factors degradation mechanism

Received: 31 July 2024

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	YANG Meng-xin
	WANG Ya-jing
	LIU Wen-jia
	HU Guang-zhi
	WU Xin-yao
	LIU Yan-fang
	ZHANG Lei

Cite this article:

YANG Meng-xin,WANG Ya-jing,LIU Wen-jia等. Comparative analysis of biochar activated peroxymonosulfate and persulfate degradation of tetracycline[J]. CHINA ENVIRONMENTAL SCIENCECE, 2025, 45(2): 810-819.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2025/V45/I2/810

[1] Daghrir R, Drogui P. Tetracycline antibiotics in the environment: a review [J]. Environmental Chemistry Letters, 2013,11(3):209-227.
[2] Gopal G, Alex S A, Chandrasekaran N, et al. A review on tetracycline removal from aqueous systems by advanced treatment techniques [J]. Rsc Advances, 2020,10(45):27081-27095.
[3] Li D, Zhang S, Li S, et al. Mechanism of the application of single-atom catalyst-activated PMS/PDS to the degradation of organic pollutants in water environment: A review[J]. Journal of Cleaner Production, 2023,397:136468.
[4] Yang Y, Banerjee G, Brudvig G W, et al. Oxidation of organic compounds in water by unactivated peroxymonosulfate [J]. Environmental Science & Technology, 2018,52(10):5911-5919.
[5] Jiang M, Lu J, Ji Y, et al. Bicarbonate-activated persulfate oxidation of acetaminophen [J]. Water Research (Oxford), 2017,116:324-331.
[6] Dou J, Cheng J, Lu Z, et al. Biochar co-doped with nitrogen and boron switching the free radical based peroxydisulfate activation into the electron-transfer dominated nonradical process [J]. Applied Catalysis. B: Environmental, 2022,301:120832.
[7] Wang R, Huang D, Liu Y, et al. Recent advances in biochar-based catalysts: Properties, applications and mechanisms for pollution remediation [J]. Chemical Engineering Journal, 2019,371:380-403.
[8] Zhu H, Guo A, Wang S, et al. Efficient tetracycline degradation via peroxymonosulfate activation by magnetic Co/N co-doped biochar: Emphasizing the important role of biochar graphitization [J]. Chemical Engineering Journal, 2022,450:138428.
[9] Zhuo S, Sun H, Wang Z, et al. A magnetic biochar catalyst with dual active sites of Fe₃C and Fe₄N derived from floc: The activation mechanism for persulfate on degrading organic pollutant [J]. Chemical Engineering Journal, 2023,455:140702.
[10] Fan X, Zhang W, Liu Y, et al. Hydrothermal synthesis of sewage sludge biochar for activation of persulfate for antibiotic removal: Efficiency, stability and mechanism [J]. Environmental Research, 2023, 218:114937.
[11] Wang S, Meng X, Yan X, et al. Iron and nitrogen modified sludge biochar efficiently activated persulfate for mineralization of sulfamethoxazole in groundwater [J]. Journal of Environmental Chemical Engineering, 2023,11(6):111319.
[12] Tan C, Lu X, Cui X, et al. Novel activation of peroxymonosulfate by an easily recyclable VC@Fe₃O₄ nanoparticles for enhanced degradation of sulfadiazine [J]. Chemical Engineering Journal, 2019, 363:318-328.
[13] Zhu S S, Li X J, Kang J, et al. Persulfate activation on crystallographic manganese oxides: Mechanism of singlet oxygen evolution for nonradical selective degradation of aqueous contaminants [J]. Environmental Science & Technology, 2019,53(1):307-315.
[14] 周舟,汤磊,赵旭强,等.阴离子对层状Mo_(2)C/过氧单硫酸盐降解氯霉素类抗生素的影响 [EB/OL]. 中国环境科学, 1-10[2024-09-18].https://doi.org/10.19674/j.cnki.issn1000-6923.20231214.001.Zhou Z, Tang L, Zhao X Q, et al. Effect of inorganic anions on the de-gradation of chloramphenicol antibiotics by layered Mo2C/ peroxonosulfate system [EB/OL]. China Environmental Science,1-10 [2024-09-18].https://doi.org/10.19674/j.cnki.issn1000-6923.20231214.001.
[15] 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.
[16] Ahmad M, Lee S S, Dou X, et al. Effects of pyrolysis temperature on soybean stover-and peanut shell-derived biochar properties and TCE adsorption in water [J]. Bioresource Technology, 2012,118:536-544.
[17] Wang J, Liao Z, Ifthikar J, et al. One-step preparation and application of magnetic sludge-derived biochar on acid orange 7removal via both adsorption and persulfate based oxidation [J]. Rsc Advances, 2017, 7(3):18696-1876.
[18] Chen L, Jiang X, Xie R, et al. A novel porous biochar-supported Fe-Mn composite as a persulfate activator for the removal of acid red 88 [J]. Separation and Purification Technology, 2020,250:117232.
[19] Kim D, Ko S. Effects of thermal modification of a biochar on persulfate activation and mechanisms of catalytic degradation of a pharmaceutical [J]. Chemical Engineering Journal, 2020,399:125377.
[20] Zhu K M, Wang X S, Geng M. Catalytic oxidation of clofibric acid by peroxydisulfate activated with wood-based biochar: Effect of biochar pyrolysis temperature, performance and mechanism [J]. Chemical Engineering Journal, 2019,374:1253-1263.
[21] Hussain I, Li M, Zhang Y, et al. Insights into the mechanism of persulfate activation with nZVI/BC nanocomposite for the degradation of nonylphenol [J]. Chemical Engineering Journal, 2017,311:163-172.
[22] Sun R, Zhang X, Wang C, et al. Co-carbonization of red mud and waste sawdust for functional application as Fenton catalyst: Evaluation of catalytic activity and mechanism [J]. Journal of Environmental Chemical Engineering, 2021,9(4):105368.
[23] Ouyang D, Chen Y, Yan J, et al. Activation mechanism of peroxymonosulfate by biochar for catalytic degradation of 1,4-dioxane: Important role of biochar defect structures [J]. Chemical Engineering Journal, 2019,370:614-624.
[24] Gong H, Chu W, Xu K, et al. Efficient degradation, mineralization and toxicity reduction of sulfamethoxazole under photo-activation of peroxymonosulfate by ferrate (VI) [J]. Chemical Engineering Journal, 2020,389:124084.
[25] Liu J, Zhu J, Zeng X, et al. Enhanced activation of persulfate by bimetal and nitrogen co-doped biochar for efficient degradation of refractory organic contaminants: The role of the second metal [J]. The Journal of Physics and Chemistry of Solids, 2024,193:112191.
[26] 贾华,牛建瑞,高玮,等.电子转移主导的载钴生物炭活化PMS降解四环素 [J]. 环境科学学报, 2024,44(3):51-60.Jia H, Niu J R, Gao W, et al. Electron transfer dominated cobalt-loaded biochar activation of PMS for tetracycline degradation [J]. Acta Scientiae Circumstantiae, 2024,44(3):51-60.
[27] He Q, Zhao C, Tang L, et al. Peroxymonosulfate and peroxydisulfate activation by fish scales biochar for antibiotics removal: Synergism of N, P-codoped biochar [J]. Chemosphere, 2023,326:138326.
[28] Huang N, Wang T, Wu Y, et al. Preparation of magnetically recyclable hierarchical porous sludge-pine needle derived biochar loaded CoFe₂O₄ nanoparticles for rapid degradation of tetracycline by activated PMS [J]. Materials Today Communications, 2023,35: 106313.
[29] Ma Y, Chen X, Tang J, et al. An in-situ electrogenerated persulfate and its activation by functionalized sludge biochar for efficient degradation of sulfamethoxazole [J]. Journal of Cleaner Production, 2023,423:138768.
[30] Fan Y, Li Y, Hayat F, et al. Multi-targeted removal of coexisted antibiotics in water by the synergies of radical and non-radical pathways in PMS activation [J]. Separation and Purification Technology, 2023,305:122475.
[31] Yang X, Duan Y, Wang J, et al. The Impact of peroxymonocarbonate (HCO₄^-) on the transformation of organic contaminants during hydrogen peroxide (H₂O₂) in situ chemical oxidation (ISCO) [J]. Environmental Science & Technology Letters, 2019,6(12):781-786.
[32] Ahn Y, Kim J, Kim K. Activation of peroxymonosulfate by bicarbonate and acceleration of the reaction by freezing [J]. Science of the Total Environment, 2021,785:147369.
[33] Diao Z, Zhang W, Liang J, et al. Removal of herbicide atrazine by a novel biochar based iron composite coupling with peroxymonosulfate process from soil: Synergistic effect and mechanism [J]. Chemical Engineering Journal, 2021,409:127684.
[34] Yang Y, Banerjee G, Brudvig G W, et al. Oxidation of organic compounds in water by unactivated peroxymonosulfate [J]. Environmental Science & Technology, 2018,52(10):5911-5919.
[35] Tang F, Dai H, Yang X, et al. Nitrogen and sulfur co-doped watermelon rind as an ordered mesoporous biochar activated peroxymonosulfate (PMS) for efficient tetracycline degradation [J]. Journal of Environmental Chemical Engineering, 2024,12(2):112302.
[36] Yang S, Yang X, Shao X, et al. Activated carbon catalyzed persulfate oxidation of azo dye acid orange 7at ambient temperature [J]. Journal of Hazardous Materials, 2011,186(1):659-666.
[37] Wei T, Meng Y, Ai D, et al. Ball milling Fe₃O₄@biochar cathode coupling persulfate for the removal of sulfadiazine from water: Effectiveness and mechanisms [J]. Journal of Environmental Chemical Engineering, 2022,10(6):108879.
[38] Xia X, Zeng S, Li K, et al. Unraveling the outstanding catalytic efficiency of unprocessed bone-derived biochar: A deep dive into the mechanisms of native organic encapsulation and defective nitrogen doping in boosting persulfate activation for tetracycline degradation [J]. Separation and Purification Technology, 2025,353:128571.
[39] Zhang Y, Xu M, Liang S, et al. Mechanism of persulfate activation by biochar for the catalytic degradation of antibiotics: Synergistic effects of environmentally persistent free radicals and the defective structure of biochar [J]. Science of the Total Environment, 2021,794:148707.
[40] Tan J Q, Chen X M, Shang M R, et al. N-doped biochar mediated peroxydisulfate activation for selective degradation of bisphenol A: The key role of potential difference-driven electron transfer mechanism [J]. Chemical Engineering Journal, 2023,468:143476.
[41] Liu Y N, Luo J, Tang L, et al. Origin of the enhanced reusability and electron transfer of the carbon-coated Mn₃O₄nanocube for persulfate activation [J]. ACS Catalysis, 2020,10(24):14857-14870.