Performance and mechanism of Cu-Mn-MRBC in the removal of ENR, STZ and TCH antibiotics from water
DONG Ying-hong1, LI Hong-yan1, CUI Jian-guo1, FENG Kun1, LI Shang-ming2, WANG Fang3,4
1. College of Environmental Science and Engineering, Taiyuan University of Technology, Shanxi Municipal Engineering Graduate Education Innovation Center, Jinzhong 030600, China; 2. College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China; 3. Research Center for Edible Fungi, Biological Institute of Shanxi Province, Taiyuan 030006, China; 4. Shanxi Key Laboratory of Edible Fungi for Loess Plateau, Taigu 030801, China
Abstract：This study aimed to investigate the mechanism of action of multiple antibiotic pollutants coexisting in water bodies. In this work, MR biochar (MRBC) was obtained through carbonization using waste bacterial residue (MR) as raw material, and Cu-Mn-MRBC was synthesized through the composite modification of both copper and manganese. The materials were characterized and analyzed by SEM, BET, XRD, FTIR, zeta potential, and EA. Furthermore, the adsorption performance of three antibiotics of ENR, STZ and TCH in single and mixed solutions was studied as well. The results show that comparing with single solution, the emergence of competitive adsorption in mixed solutions increases the selective depletion of oxygen-containing functional groups. Moreover, it promotes the adsorption of TCH with the removal rate of 96.50% in the mixed solution, but inhibits STZ more than ENR, with the removal rates in the mixed solution of 39.38% and 46.13%, respectively. Absorption process in the system decreased the pH dependence. The presence of coexisting cations affects the competitive adsorption capacity of antibiotics. Pseudo-second-order kinetic and Freundlich isotherm models can better describe the adsorption process of Cu-Mn-MRBC. The adsorption is mainly the results of electrostatic interaction, π-π interaction, hydrogen bonding, and surface complexation.
董颖虹, 李红艳, 崔建国, 冯坤, 李尚明, 王芳. Cu-Mn-MRBC去除水中ENR、STZ及TCH抗生素的性能与机理[J]. 中国环境科学, 2022, 42(12): 5668-5678.
DONG Ying-hong, LI Hong-yan, CUI Jian-guo, FENG Kun, LI Shang-ming, WANG Fang. Performance and mechanism of Cu-Mn-MRBC in the removal of ENR, STZ and TCH antibiotics from water. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(12): 5668-5678.
Fan X, Qian Z, J Liu, et al. Investigation on the adsorption of antibiotics from water by metal loaded sewage sludge biochar[J]. Water Science & Technology, 2020,83(26):739-750.
[2]
Chu L, Chen D, Wang J, et al. Degradation of antibiotics and inactivation of antibiotic resistance genes (ARGs) in Cephalosporin C fermentation residues using ionizing radiation, ozonation and thermal treatment[J]. Journal of Hazardous Materials, 2019,382:121058.
[3]
O'Neill, J. Antimicrobial Resistance:Tackling a crisis for the health and wealth of nations[R]. London:Review on Antimicrobial Resistance, 2014.
[4]
Ahmed M B, Zhou J L, Ngo H H, et al. Progress in the preparation and application of modified biochar for improved contaminant removal from water and wastewater[J]. Bioresource Technology, 2016,214:836-851.
[5]
Rahmani A R, D Nematollahi, Samarghandi M R, et al. A combined advanced oxidation process:Electrooxidation-ozonation for antibiotic ciprofloxacin removal from aqueous solution[J]. Journal of Electroanalytical Chemistry, 2018,808:82-89.
[6]
Qin P, Huang D, Tang R, et al. Enhanced adsorption of sulfonamide antibiotics in water by modified biochar derived from bagasse[J]. Open Chemistry, 2019,17(1):1309-1316.
[7]
Hu X, Hu X, Peng Q, et al. Mechanisms underlying the photocatalytic degradation pathway of ciprofloxacin with heterogeneous TiO2[J]. Chemical Engineering Journal, 2019,380(3):122366.
[8]
Yin Q, Wang R, Zhao Z. Application of Mg-Al-modified biochar for simultaneous removal of ammonium, nitrate, and phosphate from eutrophic water[J]. Journal of Cleaner Production, 2018,176:230-240.
[9]
Kosik P K, Bo P, Yong S O, et al. Engineered biochar-a sustainable solution for the removal of antibiotics from water[J]. Chemical Engineering Journal, 2020,405:126926.
[10]
Jin E, Lee S, Kang E, et al. Metal-organic frameworks as advanced adsorbents for pharmaceutical and personal care products[J]. Coordination Chemistry Reviews, 2020,425:213526.
[11]
Liu M K, Liu Y Y, Bao D D, et al. Effective removal of tetracycline antibiotics from water using hybrid carbon membranes[J]. Scientific Reports, 2017,7:43717.
[12]
Li M F, Liu Y G, Zeng G M, et al. Graphene and graphene-based nanocomposites used for antibiotics removal in water treatment:A review[J]. Chemosphere, 2019,226:360-380.
[13]
Gan X, Chen L, Chen X, et al. Agricultural bio-waste for removal of organic and inorganic contaminants from waste diesel engine oil[J]. Journal of Hazardous Materials, 2021,414:124906.
[14]
Mo J, Yang Q, Zhang N, et al. A review on agro-industrial waste (AIW) derived adsorbents for water and wastewater treatment-ScienceDirect[J]. Journal of Environmental Management, 2018,227:395-405.
[15]
Shen Q, Wang Z, Yu Q, et al. Removal of tetracycline from an aqueous solution using manganese dioxide modified biochar derived from Chinese herbal medicine residues[J]. Environmental Research, 2020, 183:109195.
[16]
Li H, Liu L, Cui J, et al. High-efficiency adsorption and regeneration of methylene blue and aniline onto activated carbon from waste edible fungus residue and its possible mechanism[J]. RSC Advances, 2020, 10:14262-14273.
[17]
范世锁,刘文浦,王锦涛,等.茶渣生物炭制备及其对溶液中四环素的去除特性.[J]. 环境科学, 2020,41(3):1308-1318. Fan S S, Liu W P, Wang J T, et al. Preparation of tea residue biochar and its removal characteristics of tetracycline in solution.[J]. Environmental Science, 2020,41(3):1308-1318.
[18]
李蕊宁.改性马铃薯秸秆生物炭对水体中典型抗生素的吸附性能研究[D]. 兰州:兰州大学, 2018. Li R N. Study on the adsorption properties of modified potato straw biochar on typical antibiotics in water[D]. Lanzhou:Lanzhou University, 2018.
[19]
Qi L, Tang X, Wang Z, et al. Pore characterization of different types of coal from coal and gas outburst disaster sites using low temperature nitrogen adsorption approach[J]. International Journal of Mining Science and Technology, 2017,27(2):371-377.
[20]
叶协锋,于晓娜,周涵君,等.不同秸秆生物炭的孔隙结构及其差异[J]. 生物质化学工程, 2019,53(2):41-46. Ye X F, Yu X N, Zhou H J, et al. Pore structure and differences of different straw biochars[J]. Biomass Chemical Engineering, 2019, 53(2):41-46.
[21]
Vadivelan V, Kumar K V. Equilibrium, kinetics, mechanism, and process design for the sorption of methylene blue onto rice husk[J]. J Colloid Interface, 2005,286(1):90-100.
[22]
Zhang C L, Qiao G L, F Zhao, et al. Thermodynamic and kinetic parameters of ciprofloxacin adsorption onto modified coal fly ash from aqueous solution[J]. Journal of Molecular Liquids, 2011,163(1):53-56.
[23]
Ahmed M B, Zhou J L, Ngo H H, et al. Single and competitive sorption properties and mechanism of functionalized biochar for removing sulfonamide antibiotics from water[J]. Chemical Engineering Journal, 2017,311:348-358.
[24]
Wang H, Fang C, Wang Q, et al. Sorption of tetracycline on biochar derived from rice straw and swine manure[J]. Rsc Advances, 2018, 8(29):16260-16268.
[25]
余剑,丁恒,张智霖,等.改性菱角壳生物炭吸附水中土霉素性能与机理[J]. 中国环境科学, 2021,41(12):5688-5700. Yu J, Ding H, Zhang Z L, et al. Performance and mechanism of modified water chestnut shell biochar for adsorption of oxytetracycline in water[J]. China Environmental Science, 2021,41(12):5688-5700.
[26]
Luo J, Li X, Ge C, et al. Sorption of norfloxacin, sulfamerazine and oxytetracycline by KOH-modified biochar under single and ternary systems[J]. Bioresource Technology, 2018,263:385-392.
[27]
Chen H, Ma L Q, Gao B, et al. Effects of Cu and Ca cations and Fe/Al coating on ciprofloxacin sorption onto sand media[J]. Journal of Hazardous Materials, 2013,252-253:375-381.
[28]
Kim J R, Kan E. Heterogeneous photocatalytic degradation of sulfamethoxazole in water using a biochar-supported TiO2 photocatalyst[J]. Journal of Environmental Management, 2016,180:94-101.
[29]
Cao J, Xiong Z, Lai B. Effect of initial pH on the tetracycline (TC) removal by zero-valent iron:Adsorption, oxidation and reduction[J]. Chemical Engineering Journal, 2018,343:492-499.
[30]
Xiang W, Wan Y, Zhang X, et al. Adsorption of tetracycline hydrochloride onto ball-milled biochar:Governing factors and mechanisms[J]. Chemosphere, 2020,255:127057.
[31]
Rajapaksha A U, Vithanage M, Ahmad M, et al. Enhanced sulfamethazine removal by steam-activated invasive plant-derived biochar[J]. Journal of Hazardous Materials, 2015,290:43-50.
[32]
S Stéphanie, Marta O L, Emmanuel G. Sorptive removal of enrofloxacin antibiotic from aqueous solution using a ligno-cellulosic substrate from wheat bran[J]. Journal of Environmental Chemical Engineering, 2018,6(5):5820-5829.
[33]
Gao M, Zhang Y, Gong X, et al. Removal mechanism of di-n-butyl phthalate and oxytetracycline from aqueous solutions by nano-manganese dioxide modified biochar[J]. Environmental Science & Pollution Research, 2018,25(8):7796-7807.
[34]
Oladipo A A, Ifebajo A O. Highly efficient magnetic chicken bone biochar for removal of tetracycline and fluorescent dye from wastewater:Two-stage adsorber analysis[J]. Journal of Environmental Management, 2017,209:9-16.
