磺化生物炭活化过硫酸盐去除水中盐酸四环素

Abstract
Figure/Table
References
Related Citation (15)

Download: PDF (1041 KB) HTML (0 KB)
Export: BibTeX | EndNote (RIS)

Abstract Sulfonated modified ramie biochar (SBC) was prepared by a high temperature calcination-sulfonation method and used as a persulfate activator to effectively remove tetracycline hydrochloride (TCH) from aqueous solutions. The morphology and structure of SBC were characterized by scanning electron microscopy (SEM), specific surface area analyzer (BET) and Fourier transform infrared spectroscopy (FT-IR). Effects of initial pH value and the dosages of SBC and PS on TCH degradation in the SBC/PS system were investigated. Also, reuse properties of synthetic materials were examined. The results showed that SBC were lamellar mesoporous materials with abundant oxygen-containing and xanthate functional groups on their surface. Under the optimal conditions of initial pH value of 3, PS dosage of 10mmol/L and SBC dosage of 0.5g/L, the TCH removal of SBC/PS system reached 89.0% after 180min, which was significantly better than that of SBC, ramie straw original biochar (BC), PS and BC/PS systems. Within the experiment scope of this investigation, the degradation performance of TCH by SBC/PS system exhibited a falling-rising-falling pattern with the increase of pH (pH=3~11). With increasing dosage of PS and SBC, the removal of TCH tended to increase, then drop. Free radical quenching experiments and electron paramagnetic resonance (EPR) experiments showed that the sulfate radical (SO₄^-·), hydroxyl radical (·OH), superoxide radical (O₂^-·) and single oxygen (¹O₂) were produced and ¹O₂ played a dominating role in the SBC/PS system during the degradation of TCH. The recycling experiments revealed that SBC had an improved reusability. This study suggested that the SBC was an environmentally friendly and efficient non-metallic carbon-based persulfate activator with a promising prospect of applications.

Key words： biochar persulfate activator tetracycline hydrochloride sulfonated modified catalytic degradation

Received: 07 January 2022

PACS:

X703

	Service

	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	DONG Kang-ni
	XIE Geng-xin
	YAN Ming
	YAN Zhuo-yi
	XIONG Xin

Cite this article:

DONG Kang-ni,XIE Geng-xin,YAN Ming等. Removal of tetracycline hydrochloride from aqueous solutions by sulfonated biochar-activated persulfate[J]. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(8): 3650-3657.

URL:

http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2022/V42/I8/3650

[1]	Ramachanderan R, Schaefer B. Tetracycline antibiotics[J]. Chemtexts, 2021,7(3):1-42.
[2]	Caco A I, Varanda F, Pratas de Melo M J P, et al. Solubility of antibiotics in different solvents. Part II. Non-hydrochloride forms of tetracycline and ciprofloxacin[J]. Industrial & Engineering Chemistry Research, 2008,47(21):8083-8089.
[3]	陈小平,王萌,杨长明,等.四环素类抗生素在我国水环境污染现状及其对水生生物的毒性研究进展[J]. 应用化工, 2021,50(10):2780-2785. Chen X P, Wang M, Yang C M, et al. Review of contaminations in water of tetracyclines in China and toxicity on aquatic organisms[J]. Applied Chemical Industry, 2021,50(10):2780-2785.
[4]	Borghi A A, Palma M A. Tetracycline:production, waste treatment and environmental impact assessment[J]. Brazilian Journal of Pharmaceutical Sciences, 2014,50(1):25-40.
[5]	Xu L Y, Zhang H, Xiong P, et al. Occurrence, fate, and risk assessment of typical tetracycline antibiotics in the aquatic environment:A review[J]. Science of the Total Environment, 2021,753:141975.
[6]	Wang D B, Jia F Y, Wang H, et al. Simultaneously efficient adsorption and photocatalytic degradation of tetracycline by Fe-based MOFs[J]. Journal of Colloid and Interface Science, 2018,519:273-284.
[7]	Ngigi A N, Ok Y S, Thiele-Bruhn S. Biochar-mediated sorption of antibiotics in pig manure[J]. Journal of Hazardous Materials, 2019, 364:663-670.
[8]	陈天民,陈颢明,马红玉,等.炭基-Co3O4复合材料活化过一硫酸盐降解阿特拉津[J]. 中国环境科学, 2020,40(11):4786-4794. Chen T M, Chen H M, Ma H Y, et al. Biochar-Co3O4 composite activates peroxymonosulfate to degrade atrazine[J]. China Environmental Science, 2020,40(11):4786-4794.
[9]	苏冰琴,刘一清,林昱廷,等.Fe3O4磁性纳米颗粒激活过硫酸盐体系同步去除水中的诺氟沙星和铅[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(Il) from aqueous solutions through Fe3O4 activated persulfate system[J]. China Environmental Science, 2022,42(2):717-727.
[10]	Tan X P, Shaaban M, Yang J W, et al. Efficient removal of hexavalent chromium from an aquatic system using nanoscale zero-valent iron supported by ramie biochar[J]. Nanomaterials, 2021,11(10):2698.
[11]	陈卫刚,武海霞,樊佳炜.活性炭非均相活化不同过硫酸盐降解偶氮染料酸性橙Ⅱ[J]. 环境工程, 2020,38(8):113-118,157. Chen W G, Wu H X, Fan J W. Activated carbon heterogeneous activation of different persulfates to degradation azo dye acid orange Ⅱ[J]. Environmental Engineering, 2020,38(8):113-118,157.
[12]	Yang Z, Zhao Z W, Yang X, et al. Xanthate modified magnetic activated carbon for efficient removal of cationic dyes and tetracycline hydrochloride from aqueous solutions[J]. Colloids and Surfaces a-Physicochemical and Engineering Aspects, 2021,615:126273.
[13]	Lv L, Chen N, Feng C P, et al. Xanthate-modified magnetic chitosan/poly (vinyl alcohol) adsorbent:Preparation, characterization, and performance of Pb(II) removal from aqueous solution[J]. Journal of the Taiwan Institute of Chemical Engineers, 2017,78:485-492.
[14]	熊道陵,李金辉,钟洪辉.应用基团电负性理论分析丙三醇黄原酸钠抑制毒砂作用机理[J]. 中南大学学报(自然科学版), 2010,41(6):2156-2161. Xiong D L, Li J H, Zhong H H. Analysis of suppression mechanism of arsenopyrite by glycerol sodium xanthogenate using group electronegatixity theory[J]. Journal of Central South University (Natural Science Edition), 2010,41(6):2156-2161.
[15]	Lau T K, Chu W, Graham N J. The aqueous degradation of butylated hydroxyanisole by UV/S2O82-:study of reaction mechanisms via dimerization and mineralization[J]. Environmental Science & Technology, 2007,41(2):613-619.
[16]	黄伟英,刘菲,鲁安怀,等.过氧化氢与过硫酸钠去除有机污染物的进展[J]. 环境科学与技术, 2013,36(9):88-95. Huang W Y, Liu F, Lu A H, et al. Removal of organic pollutants by hydrogen peroxide and sodium persulfate:a review[J]. Environmental Science & Technology, 2013,36(9):88-95.
[17]	杨珂,唐琪,杨晓丹,等.铁酸铜非均相活化过硫酸盐降解罗丹明B[J]. 中国环境科学, 2019,39(9):3761-3769. Yang K, Tang Q, Yang X D, et al. Degradation of rhodamine B by heterogeneous activation of persulfate with copper ferrate[J]. China Environmental Science, 2019,39(9):3761-3769.
[18]	Zhu K, Shen Y Q, Hou J M, et al. One-step synthesis of nitrogen and sulfur co-doped mesoporous graphite-like carbon nanosheets as a bifunctional material for tetracycline removal via adsorption and catalytic degradation processes:Performance and mechanism[J]. Chemical Engineering Journal, 2021,412:128521.
[19]	曾令泽,高鸿慈.关于四环素类药物pKa值的讨论[J]. 中国药学杂志, 1987,22(1):56. Zeng L Z, Gao H C. Discussion on pKa value of tetracycline drugs[J]. Chinese Pharmaceutical Journal, 1987,22(1):56.
[20]	李宗宸,魏群山,罗专溪,等.水土比、pH和有机质对沉积物吸附四环素的复合影响[J]. 农业环境科学学报, 2017,36(4):761-767. Li Z C, Wei Q S, Luo Z X, et al. Combination effects of pH, solution/soil ratio and inherent organic matter on the adsorption of tetracycline by sediments[J] Journal of Agro-Environment Science, 2017,36(4):761-767.
[21]	李国亭,李康丽,张帅阳,等.木质纤维素生物炭对亚甲基蓝和四环素的吸附对比研究[J]. 江苏农业科学, 2021,49(18):234-240. Li G T, Li K L, Zhang S Y, et al. Comparative study on adsorption of methylene blue and tetracycline by lignocellulosic biochar[J]. Jiangsu Agricultural Sciences, 2021,49(18):234-240.
[22]	Rao L J, Yang Y F, Liu X D, et al. Heterogeneous activation of persulfate by supporting ferric oxalate onto activated carbon fibers for organic contaminants removal[J]. Materials Research Bulletin, 2020, 130:110919.
[23]	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/Fe-MOFs/persulfate system[J]. China Environmental Science, 2021,41(6):2685-2697.
[24]	周阳,应路瑶,于欣,等.碱热联合活化过硫酸钠氧化降解2,4-二氯苯酚研究[J]. 水处理技术, 2021,47(3):68-72. Zhou Y, Ying L Y, Yu X, et al. Study on oxidative degradation of 2,4-Dichlorophenol by alkaline and thermal Co-activated sodium persulfate[J]. Technology of Water Treatment, 2021,47(3):68-72.
[25]	Furman O S, Teel A L, Ahmad M, et al. Effect of Basicity on Persulfate Reactivity[J]. Journal of Environmental Engineering-Asce, 2011,137(4):241-247.
[26]	Guan Y H, Ma J, Ren Y M, et al. Efficient degradation of atrazine by magnetic porous copper ferrite catalyzed peroxymonosulfate oxidation via the formation of hydroxyl and sulfate radicals[J]. Water Research, 2013,47(14):5431-5438.
[27]	朱紫琦,李立,徐铭骏,等.菱形片状铁锰催化剂活化过硫酸盐降解四环素[J]. 中国环境科学, 2021,41(11):5142-5152. Zhu Z Q, Li L, Xu M J, et al. Rhombic sheet iron-maganese catalyst-activating peroxymonosulfate for tetracycline degradation[J]. China Environmental Science, 2021,41(11):5142-5152.
[28]	Li J, Ren Y, Ji F Z, et al. Heterogeneous catalytic oxidation for the degradation of p-nitrophenol in aqueous solution by persulfate activated with CuFe2O4 magnetic nano-particles[J]. Chemical Engineering Journal, 2017,324:63-73.
[29]	杨奕飞,杨天学,吴代赦,等.改性沼渣生物质炭活化过硫酸盐降解酚类性能[J]. 中国环境科学, 2022,42(5):2153-2160. Yang Y F, Yang T X, Wu D M, et al. Study on the performance of modified biogas residue biomass charcoal to activate persulfate to degradation phenals[J]. China Environmental Science, 2022,42(5):2153-2160.
[30]	Shao F L, Wang Y J, Mao Y R, et al. Degradation of tetracycline in water by biochar supported nanosized iron activated persulfate[J]. Chemosphere, 2020,261:127844.
[31]	Cui Q T, Zhang W, Chai S Y, et al. The potential of green biochar generated from biogas residue as a heterogeneous persulfate activator and its non-radical degradation pathways:Adsorption and degradation of tetracycline[J]. Environmental Research, 2022,204:112335.
[32]	Guo Y P, Zeng Z Q, Li Y L, et al. In-situ sulfur-doped carbon as a metal-free catalyst for persulfate activated oxidation of aqueous organics[J]. Catalysis Today, 2018,307:12-19.
[33]	李凯,刘新璐,李辉,等.狐尾藻生物炭活化过硫酸盐降解四环素的研究[J]. 环境科学与技术, 2021,44(6):50-57. Li K, Liu X L, Li H, et al. Research of tetracycline degradation by persulfate activated with myriophyllum spicatum biochar[J]. Environmental Science & Technology, 2021,44(6):50-57.
[34]	Xia D H, Yin R, Sun J L, et al. Natural magnetic pyrrhotite as a high-Efficient persulfate activator for micropollutants degradation:Radicals identification and toxicity evaluation[J]. Journal of Hazardous Materials, 2017,340:435-444.
[35]	Cheng X, Guo H G, Zhang Y L, et al. Non-photochemical production of singlet oxygen via activation of persulfate by carbon nanotubes[J]. Water Research, 2017,113:80-88.
[36]	Tang L, Yu J F, Pang Y, et al. Sustainable efficient adsorbent:Alkali-acid modified magnetic biochar derived from sewage sludge for aqueous organic contaminant removal[J]. Chemical Engineering Journal, 2018,336:160-169.
[37]	Xiang Y J, Xu Z Y, Wei Y Y, et al. Carbon-based materials as adsorbent for antibiotics removal:Mechanisms and influencing factors[J]. Journal of Environmental Management, 2019,237:128-138.
[38]	Kamagate M, Assadi A A, Kone T, et al. Activation of persulfate by irradiated laterite for removal of fluoroquinolones in multi-component systems[J]. Journal of Hazardous Materials, 2018,346:159-166.