Efficient removal of sulfadiazine by water hyacinth
ZHANG Yue, YUAN Yu-long, YAN Cai-xia, JIANG Yi-han, SU Mei-qi, DING Ming-jun, WANG Peng, NIE Ming-hua
Key Laboratory of Poyang Lake Wetland and Watershed Research, Ministry of Education, Jiangxi Province Key Laboratory of Ecological Intelligent Monitoring and Comprehensive Treoctment of Watershed, School of Geography and Environment, Jiangxi Normal University, Nanchang 330022, China
Abstract：Water hyacinth biochar (EBC), derived from the invasive plant water hyacinth, exhibited remarkable capabilities in activating periodate (PI) and facilitating the degradation of sulfadiazine (SD). Notably, EBC outperformed Alligator weed BC and Canadian goldenrod BC in this regard. Among various pyrolysis temperatures, EBC prepared at 500℃(EBC500) demonstrated superior PI activation, effectively removing SD within a mere 20 minutes using a lower PI dose (0.15mmol/L). As the dosage of EBC500 and PI increased, the removal rate of SD also increased accordingly. Comprehensive analyses, including bursting experiments and electron paramagnetic resonance analysis, revealed that iodine radicals (×IO3, ×IO4), superoxide radicals (O2•−), and singlet oxygen (1O2) served as the primary reactive species responsible for the degradation of SD in the EBC500/PI system. Meanwhile, under the conditions of EBC500 and PI dosages of 0.15g/L and 0.15mmol/L, respectively, SD can be completely removed across a wide range of initial pH values (5~9). Coexisting substances such as common anions (including Cl−, SO42−, and NO3−) had minimal impact on the degradation of SD in the EBC500/PI system. However, HCO3− and HA exhibited inhibitory effects on the removal of SD. Moreover, the EBC500/PI system demonstrates robust applicability for the degradation of SD in natural water matrixes, and good application potential for degradation of other typical sulfonamide antibiotics as well. Additionally, EBC500 demonstrated favorable reusability. Based on the identification of six intermediates, potential degradation pathways of SD were proposed. Ecotoxicity analysis and plant seed germination tests confirmed that the treatment with the EBC500/PI system significantly reduced the biological toxicity of SD, underscoring its promising application prospects.
[1] Yang S, Shi Y, Wang X H, et al. Selective elimination of sulfonamide antibiotics upon periodate/catechol process: Dominance of quinone intermediates [J]. Water Research, 2023,242:120317. [2] Wang B, Ni B-J, Yuan Z, et al. Insight into the nitrification kinetics and microbial response of an enriched nitrifying sludge in the biodegradation of sulfadiazine [J]. Environmental Pollution, 2019,255:113160. [3] 时红蕾,王晓昌,李倩.人粪便好氧堆肥过程中典型抗生素的消减特性[J]. 环境科学, 2018,39(7):3434-3442. Shi H L, Wang X C, Li Q. Abatement characteristics of typical antibiotics during aerobic composting of human waste [J]. Environmental Science, 2018,39(7):3434-3442. [4] Bielen A, Šimatović A, Kosić-Vukšić J, et al. Negative environmental impacts of antibiotic-contaminated effluents from pharmaceutical industries [J]. Water Research, 2017,126:79-87. [5] Chen J, Xie S. Overview of sulfonamide biodegradation and the relevant pathways and microorganisms [J]. Science of the Total Environment, 2018,640:1465-1477. [6] 石秋俊,刘安迪,唐柏彬,等.Ni掺杂Sb-SnO2瓷环粒子电极电催化氧化磺胺嘧啶[J]. 环境科学, 2020,41(4):1725-1733. Shi Q J, Liu A D, Tang B B, et al. Electrocatalytic oxidation of sulfadiazine at Ni-doped Sb-SnO2 porcelain ring particle electrode [J]. Environmental Science, 2020,41(4):1725-1733. [7] Dai J, Wang Z Q, Chen K W, et al. Applying a novel advanced oxidation process of biochar activated periodate for the efficient degradation of bisphenol A: Two nonradical pathways [J]. Chemical Engineering Journal, 2023,453:139889. [8] Chen T S, Sun Y K, Dong H Y, et al. Understanding the importance of periodate species in the pH-dependent degradation of organic contaminants in the H2O2/periodate process [J]. Environmental Science & Technology, 2022,56(14):10372-10380. [9] Zong Y, Shao Y, Zeng Y, et al. Enhanced oxidation of organic contaminants by iron (II)-activated periodate: The significance of high-valent iron–oxo species [J]. Environmental Science & Technology, 2021,55(11):7634-7642. [10] He L Y, Lv L X, Pillai S C, et al. Efficient degradation of diclofenac sodium by periodate activation using Fe/Cu bimetallic modified sewage sludge biochar/UV system [J]. Science of the Total Environment, 2021,783:146974. [11] Choi Y, Yoon H I, Lee C, et al. Activation of periodate by freezing for the degradation of aqueous organic pollutants [J]. Environmental Science & Technology, 2018,52(9):5378-5385. [12] Hamdaoui O, Merouani S. Improvement of sonochemical degradation of Brilliant blue R in water using periodate ions: Implication of iodine radicals in the oxidation process [J]. Ultrasonics Sonochemistry, 2017,37:344-350. [13] Bokare A D, Choi W. Singlet-oxygen generation in alkaline periodate solution [J]. Environmental Science & Technology, 2015,49(24): 14392-14400. [14] Zong Y, Shao Y, Zeng Y, et al. Enhanced oxidation of organic contaminants by iron (II)-activated periodate: The significance of high-valent iron–oxo species [J]. Environmental Science & Technology, 2021,55(11):7634-7642. [15] Lee H, Yoo H Y, Choi J, et al. Oxidizing capacity of periodate activated with iron-based bimetallic nanoparticles [J]. Environmental Science & Technology, 2014,48(14):8086-8093. [16] Cai S, Zhang Q, Wang Z, et al. Pyrrolic N-rich biochar without exogenous nitrogen doping as a functional material for bisphenol A removal: Performance and mechanism [J]. Applied Catalysis B: Environmental, 2021,291:120093. [17] Yan J, Zuo X, Yang S, et al. Evaluation of potassium ferrate activated biochar for the simultaneous adsorption of copper and sulfadiazine: Competitive versus synergistic [J]. Journal of Hazardous Materials, 2022,424:127435. [18] 相里鹏,崔佳丽,张峰,等.磁性生物炭活化过硫酸盐去除水中罗丹明B [J]. 中国环境科学, 2023,43(4):1672-1687. Xiang L P, Cui J L, Zhang F, et al. Removal of rhodamine B from water by magnetic biochar activated persulfate [J]. China Environmental Science, 2023,43(4):1672-1687. [19] 姚淑华,马锡春,李士凤.秸秆生物炭活化过硫酸盐氧化降解苯酚[J]. 中国环境科学, 2018,38(11):4166-4172. Yao S H, Ma X C, Li S F. Oxidative degradation of phenol by straw biochar activated persulfate [J]. China Environmental Science, 2018, 38(11):4166-4172. [20] 李鑫,尹华,罗昊昱,等.磁性生物炭负载α-MnO2活化过一硫酸盐降解2,2',4,4'-四溴联苯醚[J]. 环境科学, 2021,42(10):4798-4806. Li X, Yin H, Luo H Y, et al. Degradation of 2,2',4,4'- tetrabromodiphenyl ether by magnetic biochar loaded α-MnO2 activated persulfate [J]. Environmental Science, 2021,42(10):4798-4806. [21] Yao Y J, Hu H H, Zheng H D, et al. Nonprecious bimetallic Fe, Mo-embedded N-enriched porous biochar for efficient oxidation of aqueous organic contaminants [J]. Journal of Hazardous Materials, 2022,422:126776. [22] He L Y, Yang S D, Shen S T, et al. Novel insights into the mechanism of periodate activation by heterogeneous ultrasonic-enhanced sludge biochar: Relevance for efficient degradation of levofloxacin [J]. Journal of Hazardous Materials, 2022,434:128860. [23] Fang G G, Li J L, Zhang C, et al. Periodate activated by manganese oxide/biochar composites for antibiotic degradation in aqueous system: Combined effects of active manganese species and biochar [J]. Environmental Pollution, 2022,300:118939. [24] Zhang X, Verbist M, Kamali M, et al. Activation of periodate with pinewood biochar-CuO composite for the removal of recalcitrant organic pollutants–Mechanisms and degradation products [J]. Chemical Engineering Journal, 2023,465:142916. [25] 周润娟,张明.水葫芦生物炭对水中重金属离子的吸附特征研究[J]. 安全与环境工程, 2022,29(3):168-177. Zhou R J, Zhang M. Adsorption characteristics of water hyacinth biochar on heavy metal ions in water [J]. Safety and Environmental Engineering, 2022,29(3):168-177. [26] Li F, He X, Shoemaker C A, et al. Experimental and numerical study of biomass catalytic pyrolysis using Ni2P-loaded zeolite: Product distribution, characterization and overall benefit [J]. Energy Conversion and Management, 2020,208:112581. [27] Lee Y, Lee S, Cui M C, et al. Activation of peroxodisulfate and peroxymonosulfate by ultrasound with different frequencies: Impact on ibuprofen removal efficient, cost estimation and energy analysis [J]. Chemical Engineering Journal, 2021,413:127487. [28] 王红,夏雯,卢平,等.生物炭对土壤中重金属铅和锌的吸附特性[J]. 环境科学, 2017,38(9):3944-3952. Wang H, Xia W, Lu P, et al. Adsorption characteristics of biochar on heavy metals lead and zinc in soil [J]. Environmental Science, 2017,38(9):3944-3952. [29] Masto R E, Kumar S, Rout T K, et al. Biochar from water hyacinth (Eichornia crassipes) and its impact on soil biological activity [J]. Catena, 2013,111:64-71. [30] 李坤权,郑正,张继彪,等.磷酸活化植物基活性炭对水溶液中铅的吸附[J]. 环境工程学报, 2010,4(6):1238-1242. Li K Q, Zheng Z, Zhang J B, et al. Adsorption of lead from aqueous solution by phosphoric acid activated plant-based activated carbon [J]. Journal of Environmental Engineering, 2010,4(6):1238-1242. [31] 徐慧敏,何国富,刘伟,等.H3PO4活化制备喜旱莲子草基活性炭及性能表征[J]. 环境工程学报, 2015,9(6):2761-2766. Xu H M, He G F, Liu W, et al. Preparation and performance characterization of Hibiscus sabdariffa-based activated carbon by H3PO4 activation [J]. Journal of Environmental Engineering, 2015,9(6): 2761-2766. [32] Lua A C, Yang T, Guo J. Effects of pyrolysis conditions on the properties of activated carbons prepared from pistachio-nut shells [J]. Journal of Analytical and Applied Pyrolysis, 2004,72(2):279–287. [33] 南志江,蒋煜峰,毛欢欢,等.玉米秸秆生物炭对灰钙土吸附金霉素的影响[J]. 环境科学, 2021,42(12):5896-5904. Nan Z J, Jiang Y F, Mao H H, et al. Effect of corn stover biochar on adsorption of chrysomycin by gray calcium soil [J]. Environmental Science, 2021,42(12):5896-5904. [34] 刘冲,吴文成,刘晓文,等.制备条件对生物质炭特性及修复重金属污染农田土壤影响研究进展[J]. 土壤, 2016,48(4):641-647. Liu C, Wu W C, Liu X W, et al. Research progress on the effect of preparation conditions on biomass char properties and remediation of heavy metal contaminated agricultural soils [J]. Soil, 2016,48(4):641-647. [35] 陈晓旋,黄晓婷,陈优阳,等.炉渣与生物炭配施对福州平原稻田土壤团聚体及碳、氮分布的影响[J]. 环境科学学报, 2018,38(5):1989-1998. Chen X X, Huang X T, Chen Y Y, et al. Effects of slag and biochar dosing on soil aggregates and carbon and nitrogen distribution in rice paddies in Fuzhou Plain [J]. Journal of Environmental Science, 2018, 38(5):1989-1998. [36] 梁欣冉,何丹,郑曌华,等.两种铁改性生物炭对微碱性砷镉污染土壤的修复效果[J]. 环境科学, 2023,44(7):4100-4108. Liang X R, He D, Zheng J H, et al. Remediation effects of two types of iron-modified biochar on slightly alkaline arsenic-cadmium contaminated soil [J]. Environmental Science, 2023,44(7):4100-4108. [37] Xiao P Y, Yi X L, Wu M H, et al. Catalytic performance and periodate activation mechanism of anaerobic sewage sludge-derived biochar [J]. Journal of Hazardous Materials, 2022,424:127692. [38] Yu J F, Tang L, Pang Y, et al. Hierarchical porous biochar from shrimp shell for persulfate activation: A two-electron transfer path and key impact factors [J]. Applied Catalysis B-Environmental, 2020,260: 118160. [39] Al-Rumaihi A, Shahbaz M, Mckay G, et al. A review of pyrolysis technologies and feedstock: A blending approach for plastic and biomass towards optimum biochar yield [J]. Renewable and Sustainable Energy Reviews, 2022,167:112715. [40] He L Y, Shi Y, Chen Y L, et al. Iron-manganese oxide loaded sludge biochar as a novel periodate activator for thiacloprid efficient degradation over a wide pH range [J]. Separation and Purification Technology, 2022,288:120703. [41] 吴承梓,张巍,万彦涛,等.盐酸羟胺/铁基MOFs/过硫酸盐体系降解磺胺嘧啶[J]. 中国环境科学, 2021,41(6):2685-2697. Wu C Z, Zhang W, Wan Y T, et al. Degradation of sulfadiazine by hydroxylamine hydrochloride/iron based MOFs/persulfate system [J]. China Environmental Science, 2021,41(6):2685-2697. [42] Zhang X, Kamali M, Yu X, et al. Kinetics and mechanisms of the carbamazepine degradation in aqueous media using novel iodate-assisted photochemical and photocatalytic systems [J]. Science of the Total Environment, 2022,825:153871. [43] Zhang Y M, Nie S H, Nie M H, et al. Remediation of sulfathiazole contaminated soil by peroxymonosulfate: Performance, mechanism and phytotoxicity [J]. Science of the Total Environment, 2022,830:154839. [44] 孙鹏佳,熊必涛,孙萍,等.双金属硫化物CoMoS4活化过一硫酸盐降解双酚F [J]. 环境科学学报, 2023,43(6):318-327. Sun P J, Xiong B T, Sun P, et al. Degradation of bisphenol F by bimetallic sulfide CoMoS4 activated peroxynitrite [J]. Journal of Environmental Science, 2023,43(6):318-327. [45] 辛丽红,晏彩霞,聂明华,等.微量铜离子联合碳酸氢盐类芬顿体系降解水中双酚A [J]. 中国环境科学, 2023,43(3):1186-1196. Xin L H, Yan C X, Nie M H, et al. Degradation of bisphenol A in water by trace copper ions combined with bicarbonate-based Fenton system [J]. China Environmental Science, 2023,43(3):1186-1196. [46] Li R, Wang J, Wu H, et al. Periodate activation for degradation of organic contaminants: Processes, performance and mechanism [J]. Separation and Purification Technology, 2022,292:120928. [47] Li X, Liu X, Lin C, et al. Enhanced activation of periodate by iodine-doped granular activated carbon for organic contaminant degradation [J]. Chemosphere, 2017,181:609-618. [48] Du J, Tang S, Faheem, et al. Insights into periodate oxidation of bisphenol A mediated by manganese [J]. Chemical Engineering Journal, 2019,369:1034-1039. [49] 陈露,蔡洁,刘夫珍,等.WS2强化Fe2+活化高碘酸盐降解酸性橙7的研究[J]. 环境科学学报, 2023,43(4):265-275. Chen L, Cai J, Liu F Z, et al. WS2 enhanced Fe2+ activated periodate degradation of acid orange 7[J]. Journal of Environmental Science, 2023,43(4):265-275. [50] Zhang N, Lin L-S, Gang D C. Adsorptive selenite removal from water using iron-coated GAC adsorbents [J]. Water Research, 2008,42(14): 3809-3816. [51] 安青,陈德珍,钦佩,等.生物炭活化技术及生物炭催化剂的研究进展[J]. 中国环境科学, 2021,41(10):4720-4735. An Q, Chen D Z, Qin P, et al. Research progress of biochar activation technology and biochar catalyst [J]. China Environmental Science, 2021,41(10):4720-4735. [52] Xu L, Xu C, Zhao M R, et al. Oxidative removal of aqueous steroid estrogens by manganese oxides [J]. Water Research, 2008,42(20): 5038-5044. [53] Liu J G, Jiang S J, Chen D D, et al. Activation of persulfate with biochar for degradation of bisphenol A in soil [J]. Chemical Engineering Journal, 2020,381:122637. [54] Fabiańska A, Bialk-Bielińska A, Stepnowski P, et al. Electrochemical degradation of sulfonamides at BDD electrode: kinetics, reaction pathway and eco-toxicity evaluation [J]. Journal of Hazardous Materials, 2014,280:579-587. [55] Yuan Y L, Nie M H, Yan C X, et al. Solar light promoted degradation of bisphenol S in carbonate/peroxymonosulfate system through accelerating singlet oxygen generation [J]. Chemical Engineering Journal, 2023,452:139153. [56] Zhou J, Ma F, Guo H, et al. Activate hydrogen peroxide for efficient tetracycline degradation via a facile assembled carbon-based composite: Synergism of powdered activated carbon and ferroferric oxide nanocatalyst [J]. Applied Catalysis B: Environmental, 2020,269:118784. [57] Yuan Y L, Wang W Y, Nie M H, et al. Visible light-mediated activation of periodate for bisphenol A degradation in the presence of Fe3+ and gallic acid at neutral pH [J]. Chemical Engineering Journal, 2024,479:147541. [58] Nie M H, Deng Y W, Nie S H, et al. Simultaneous removal of bisphenol A and phosphate from water by peroxymonosulfate combined with calcium hydroxide [J]. Chemical Engineering Journal, 2019,369:35-45.
