Research progress on activated persulfate degradation of antibiotics by magnetic biochar composites
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摘要: 抗生素具有高水溶性、高化学稳定性、潜在致癌性、明显的生态毒性和难以生物降解等特点，对水环境的可持续性和人类健康构成了严重威胁。因此，建立有效的去除水中的抗生素污染物的方法至关重要。磁性生物炭复合材料因其优异的过硫酸盐活化催化能力和可回收性，在抗生素污染物的氧化降解方面受到广泛关注。本文综述了磁性生物炭复合材料活化过硫酸盐降解抗生素的研究进展。首先，我们总结了不同生物质来源的磁性生物炭复合材料及其常用制备方法。然后，探讨了磁性生物炭复合材料活化过硫酸盐降解抗生素类污染物的机制及其对不同类型抗生素的降解行为。最后，针对目前抗生素污染引起的其他问题，提出了未来研究的挑战和展望。Abstract: Antibiotics, which have high water solubility, high chemical stability, potential carcinogenicity, obvious ecotoxicity, and difficult biodegradation, pose a serious threat to the sustainability of the aquatic environment and human health. Therefore, it is crucial to establish effective methods to remove antibiotic contaminants from water. Magnetic biochar composites have attracted much attention in the oxidative degradation of antibiotic contaminants due to their excellent catalytic capacity for activation of persulfate and recyclability. In this review, we aim to summarize the research progress of magnetic biochar composites activated persulfate degradation of antibiotics. First, we summarize magnetic biochar composites from different biomass sources and their commonly prepared methods. Then, the mechanism of activated persulfate degradation of antibiotic pollutants by magnetic biochar composites and their degradation behaviors for different types of antibiotics were explored. Finally, the challenges and prospects for future research are proposed in response to other current issues arising from antibiotic contamination.
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Key words:
- magnetic biochar /
- antibiotics /
- persulfate /
- preparation method /
- degradation mechanism
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图 1 磁性生物炭复合材料活化过硫酸盐(PS)降解抗生素的研究进展
Figure 1. Research progress on activated persulfate (PS) degradation of antibiotics by magnetic biochar composites
图 2 磁性生物炭复合材料活化PS降解抗生素的机制。
Figure 2. Mechanism of magnetic biochar composite activated persulfate to degrade antibiotics.
图 3 (a) 竹子制备的MMBC用于TC的降解；(b) MMBC活化PS的ESR谱； (c)TC的降解过程；(d)PS在MMBC上活化降解TC的主要催化机制[40]。
Figure 3. (a) MMBC prepared from bamboo for TC degradation; (b) ESR spectra of PS activation by MMBC; (c) Proposed degradation process of TC; (d)Main catalytic mechanism of PS activation on MMBC for TC degradation[40].
图 4 (a) LBC、Fe2O3和Fe2O3@LBC对CEX的去除；(b) Fe2O3@LBC/PS体系中的EPR谱；(c)Fe2O3@LBC活化PS降解CEX的可能机制；(d)降解CEX的反应途径[35]。
Figure 4. (a) The removal of CEX by LBC, Fe2O3 and Fe2O3@LBC; (b) DMPO spin trapping EPR spectra in the Fe2O3@LBC/PS system; (c) Possible mechanism of persulfate activation by Fe2O3@LBC for CEX degradation; (d) Proposed reaction pathway for the degradation of CEX[35].
图 5 (a) 生物炭负载磁性MIL-53-Fe衍生物作为过硫酸氢盐活化降解抗生素的有效催化剂。(b) NOR的降解转化途径。(c) 1.0-BC@FexC/PDS同时去除NOR的可能反应机制[41]。
Figure 5. (a) Biochar supported magnetic MIL-53-Fe derivatives as an efficient catalyst for peroxydisulfate activation towards antibiotics degradation. (b) the proposed transformation pathways of NOR degradation.(c) The possible reaction mechanism for the simultaneous removals of NOR by the 1.0-BC@FexC/PDS process[41].
图 6 (a) CoFe2O4/BC/PMS/SMX体系可能的催化降解机制；SO4•−和 HO• (b)， 1O2 (c) 在不同体系中的EPR谱；(d) SMX在CoFe2O4/BC/PMS体系中可能的降解途径[27]。
Figure 6. (a) The possible catalytic degradation mechanism over CoFe2O4/BC/PMS/SMX system; EPR spectra of SO4•−and HO• (b), 1O2 (c) in different systems; (d) The possible degradation pathways of SMX in the CoFe2O4/BC/PMS system[27].
表 1 不同生物质来源制备的磁性生物炭复合材料的催化性能
Table 1. Catalytic properties of magnetic biochar materials prepared from different biomass sources
Magnetic biochar Source Magnetic
substancePreparation method PS Antibiotics Active substance Removal efficiency Reference Magnetic rape straw biochar Rape straw Fe3O4 Pyrolysis PDS TC SO4•−、HO•、O2•−and 1O2 99.0% [26] CoFe2O4/biochar Rape straw CoFe2O4 Solvothermal PMS SMX SO4•−、HO•、O2•−and 1O2 93.0% [27] Magnetic biochar Rice straw Fe3C
Fe4NPyrolysis PDS TC SO4•−、HO•、O2•−and 1O2 90.5% [28] Coral reef-like FeS2/biochar Corn stalks FeS2 Solvothermal PMS TC SO4•−、HO•、O2•−and 1O2 100.0% [29] Modified red mud biochar Corn straw Fe3O4 Pyrolysis PDS LFX SO4•− and HO• 88.6% [30] Fe3O4 supported by N-doped biochar Corncob Fe3O4
ZnFe2O4Coprecipitation PDS TC SO4•−、HO•、O2•− and 1O2 91.6% [31] Nitrogen-doped magnetic carbon nanotubes-bridged biochar Rice husk Fe3O4 Impregnation-
pyrolysisPMS SMX SO4•−、HO• and 1O2 98.2% [32] Magnetic iron-char composites Peanut shells Fe3O4 Impregnation-
pyrolysisPDS SMX SO4•−、HO•、O2•−and 1O2 99.4% [33] FeS@biochar Peanut shells FeS Pyrolysis PDS SMT SO4•−、HO• and 1O2 96.4% [34] Magnetic loofah biochar Loofah Fe2O3 Impregnation-
pyrolysisPDS CEX SO4•− and HO• 73.9% [35] Cobalt and iron coloaded pomelo peel biochar composite; Pomelo peels CoFe2O4 Impregnation and
coprecipitationPMS TC SO4•−、HO•、O2•− and 1O2 86.2% [36] MgFe2O4/biochar Pomelo peels MgFe2O4 Coprecipitation PDS LFX O2•−and 1O2 87.9% [37] MnFe2O4/biochar Banana
pseudo-stemMnFe2O4 Sol-gel pyrolysis PDS TC SO4•−、HO•、O2•−and 1O2 94.7% [38] Lanthanum-doped magnetic biochar Bagasse Fe3O4 Impregnation-
pyrolysisPDS FLO SO4•−、HO•、O2•−and 1O2 99.5% [39] Mn doped magnetic biochar; Bamboo Fe3O4、Fe3C
And MnFe2O4Impregnation-
pyrolysisPDS TC SO4•− and HO• 93.0% [40] Biochar-loaded MIL-53(Fe) derivatives Bamboo Fe3O4、Fe0 and α-Fe2O3 Pyrolysis PDS NOR SO4•−、HO• and 1O2 91.2% [41] FeS@biochar Pine sawdust FeS Ball milling PDS TC SO4•− and HO• 87.4% [42] Potassium-doped magnetic
biocharPine sawdust Fe3O4
α-Fe2O3Impregnation-
pyrolysisPDS MNZ SO4•−、HO•、O2•−and 1O2 98.4% [43] Mn-based magnetic biochar Pine sawdust Fe3O4 Impregnation-
pyrolysisPDS MNZ SO4•−、HO•、O2•−and 1O2 95.6% [44] Nitrogen-rich magnetic
biocharPine sawdust Fe3O4
α-Fe2O3Impregnation-
pyrolysisPDS MNZ SO4•−、HO•、O2•−and 1O2 99.6% [45] CoFe2O4/biochar Sludge/pine
needleCoFe2O4 Hydrothermal PMS TC SO4•−and HO• 99.8% [46] Magnetic N-doped iron sludge based biochar Sycamore leaves and sludge Fe3O4 Pyrolysis PDS TC SO4•−、HO• and 1O2 86.6% [47] MnFe2O4/biochar Eichhornia crassipes MnFe2O4 Coprecipitation PMS TC
SMXSO4•−、HO• and 1O2 90.1%
96.5%[48] Co/N co-doped biochar Kelp Co Pyrolysis PMS TC SO4•−、HO• and 1O2 99.0% [49] Copper doping in magnetic
biocharCow dung Fe3O4 Impregnation-
pyrolysisPMS SMX
CIPSO4•−、HO•、O2•−and 1O2 91.7%
97.3%[21] Magnetic biochar Piggery sludge Fe3O4
α-Fe2O3Coprecipitation PMS TC SO4•−、HO•、O2•−and 1O2 77.2% [50] Fe/Mn bimetal co-functionalized sludge biochar Sludge Fe3O4 Impregnation-
pyrolysisPDS SMX 1O2 98.8% [51] Magnetic nitrogen-doped
sludge-derived biocharSludge γ-Fe2O3 Pyrolysis PDS TC SO4•− and HO• 82.2% [52] N-functionalized sewage sludge -red mud complex biochar Sludge Fe3O4 Pyrolysis PMS SMX SO4•−、HO•、O2•−and 1O2 97.5% [53] Co-Fe/SiO2 Iron sludge Co-Fe-LBH Solvothermal PMS CIP SO4•− and HO• 98.0% [54] Iron-loaded biochar Fermentation dreg Fe3O4 Coprecipitation PDS TC SO4•−、HO•、O2•−and 1O2 85.1% [55] Notes: LBH-layered double hydroxide; PS-persulfate； PMS-peroxymonosulfate； PDS-peroxysulphate； TC-Tetracycline; SMX-Sulfamethoxazole; SMT-Sulfamethazine; CEX-Cephalexin; LFX-Levofloxacin; FLO-Florfenicol; NOR-Norfloxacin; MNZ-Metronidazole; CIP-Ciprofloxacin. 
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表 2 不同制备磁性生物炭复合材料方法的优点和缺点
Table 2. Advantages and disadvantages of different preparation methods
Preparation method Advantage Disadvantage Reference Impregnation-pyrolysis Magnetization and pyrolysis at the same time, simple operation Gas pollutants are easy to cause secondary pollution, high temperature energy-consuming crystallinity, size and porosity are difficult to control [25,57-59] Coprecipitation Simple operation, controlled reaction The introduction of alkaline reagents is required, and the usable surface area of the prepared material is small. [60,61] Hydrothermal Low temperatures (100 ~ 300°C), mild reaction conditions, no need for bases or strong reducing agents, no need for energy-intensive pre-drying processes Higher dependence on production equipment [18,22,62,63] Chemical reduction Convenient operation, controllable reaction,
high product purityReducing agents added are toxic and need to be stored and used properly. [64]
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