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Characteristics of Cu(II)-modified aerobic granular sludge biocarbon in removal of doxycycline hydroxide

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Abstract

In this study, the biocarbon derived from aerobic granular sludge with different nutritive proportions was modified by Cu(NO3)2•3H2O (Cu-BC) to improve its adsorption capacity of doxycycline hydrochloride (DOX). The surface area, pores, functional groups, and element composition of biocarbon were characterized by scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) surface area, X-ray photoelectron spectrometer, X-ray diffraction (XRD), the X-ray photoelectron spectrometer, and Fourier transform infrared spectrometry (FT-IR), respectively. Effects of DOX concentration, initial pH, and background electrolyte on adsorption effects of composite were analyzed. Furthermore, the adsorption kinetics, isotherm, thermodynamics, and diffusion model were investigated. Results demonstrated that biocarbons which were prepared with aerobic granular sludge under different nutritive proportions presented different performances. The BET specific surface area of Cu-NaAC/AGS-BC was 260.1592 m2/g, and the micropore volume was 0.054101 cm3/g. The BET specific surface area of Cu-GLC /AGS-BC was only 10.6821 m2/g, and the micropore volume was 0.008687 cm3/g. Both kinds of modified biochar contain a large number of oxygen-containing functional groups. The highest adsorption efficiency of Cu-BC could reach 99.54%. The adsorption of DOX on two modified biocarbons conforms to the pseudo-second-order dynamic model and Temkin isothermal model.

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References

  • Ahmad T, Danish M (2018) Prospects of banana waste utilization in wastewater treatment: a review. J Environ Manag 206:330–348

    CAS  Google Scholar 

  • Ahmed MB, Zhou JL, Ngo HH, Guo WJS (2015) Adsorptive removal of antibiotics from water and wastewater. Progress and challenges. Sci Total Environ 532(nov.1):112–126

    Article  CAS  Google Scholar 

  • Amorim CL, Alves M, Castro PML, Henriques IJEES (2017) Bacterial community dynamics within an aerobic granular sludge reactor treating wastewater loaded with pharmaceuticals. Ecotoxicol Environ Saf 147(jan):905–912

    Google Scholar 

  • Aydin S, Ince B, Cetecioglu Z, Ozbayram EG, Shahi A, Okay O, Arikan O, Ince O (2014) Performance of anaerobic sequencing batch reactor in the treatment of pharmaceutical wastewater containing erythromycin and sulfamethoxazole mixture. Water Science & Technology A Journal of the International Association on Water Pollution Research 70(10):1625–1632

  • Bao Y, Zhou Q, Wan Y, Yu Q, Xie XJSSSAJ (2010) Effects of soil/solution ratios and cation types on adsorption and desorption of tetracycline in soils. Soil Sci Soc Am J 74:1553–1561

    Article  CAS  Google Scholar 

  • Chen Y, de Oliveira, Letuzia M et al (2017) Mechanisms of metal sorption by biochars: biochar characteristics and modifications. Chem Environ Toxicol Risk Assess 178(Jul.):466–478

  • Chen T, Ling L, Deng S, Shi G, Zhang S, Zhang Y et al (2018) Sorption of tetracycline on h3po4 modified biochar derived from rice straw and swine manure. Bioresour Technol 267:431–437

    Article  CAS  Google Scholar 

  • Cui L, Xu W, Guo X, Zhang Y, Wei Q, Du BJJML (2014) Synthesis of strontium hydroxyapatite embedding ferroferric oxide nano-composite and its application in Pb2+ adsorption. J Mol Liq 197:40–47

    Article  CAS  Google Scholar 

  • Danish M, Hashim R, Mohamad Ibrahim MN, Sulaiman O (2013) Effect of acidic activating agents on surface area and surface functional groups of activated carbons produced from acacia mangium wood. J Anal Appl Pyrolysis 104:418–425

    Article  CAS  Google Scholar 

  • Danish M, Ahmad T, Hashim R, Said N, Akhtar MN, Mohamad-Saleh J et al (2018) Comparison of surface properties of wood biomass activated carbons and their application against rhodamine b and methylene blue dye. Surf Interfaces:1–13

  • Dong W, Ngo HH, Guo W, Xu W, Du B, Khan MS et al (2017) Biosorption performance evaluation of heavy metal onto aerobic granular sludge-derived biochar in the presence of effluent organic matter via batch and fluorescence approaches. Annals of Hepatology Official Journal of the Mexican Association of Hepatology 16(6)

  • Fey TK, Cho YD, Chen CL, Lin YY, Kumar TP, Chan SH (2010) Pyrolytic carbons from acid/base-treated rice husk as lithium-insertion anode materials. Pure Appl Chem 82(11):2157–2165

    Article  CAS  Google Scholar 

  • Gao Y, Yan L, Liang Z, Huang H, Hu J, Shah SM et al (2012) Adsorption and removal of tetracycline antibiotics from aqueous solution by graphene oxide. J Colloid Interface Sci 368(1):540–546

    Article  CAS  Google Scholar 

  • Hai L, Liu W, Jian Z, Zhang C, Ren L, Ye L (2011) Removal of cephalexin from aqueous solutions by original and cu(ii)/fe(iii) impregnated activated carbons developed from lotus stalks kinetics and equilibrium studies. J Hazard Mater 185(2-3):1528–1535

    Article  Google Scholar 

  • Huang X, Liu Y, Liu S, Tan X, Yang D, Zeng G et al (2015) Effective removal of cr(vi) using β-cyclodextrin–chitosan modified biochars with adsorption/reduction bifuctional roles. RSC Adv 6

  • Huber MM, GöBel A, Joss A, Hermann N, LöFfler D, Mcardell CS et al (2005) Oxidation of pharmaceuticals during ozonation of municipal wastewater effluents: a pilot study. Environ Sci Technol 39(11):4290–4299

    Article  CAS  Google Scholar 

  • Jiang LH, Liu YG, Zeng GM et al (2016) Removal of 17 beta-estradiol by few-layered graphene oxide nanosheets from aqueous solutions: external influence and adsorption mechanism. Chem Eng J 284:93–102

    Article  CAS  Google Scholar 

  • Kim J, Hyun S (2018) Sorption of ionic and nonionic organic solutes onto giant miscanthus-derived biochar from methanol-water mixtures. Sci Total Environ 615(FEB.15):805–813

    Article  CAS  Google Scholar 

  • Kim H, Hwang YS, Sharma VK (2014) Adsorption of antibiotics and iopromide onto single-walled and multi-walled carbon nanotubes. Chem Eng J 255(6):23–27

    Article  CAS  Google Scholar 

  • Kümmerer K (2009) The presence of pharmaceuticals in the environment due to human use – present knowledge and future challenges. J Environ Manag 90(8):2354–2366. https://doi.org/10.1016/j.jenvman.2009.01.023

    Article  CAS  Google Scholar 

  • Li Z, Schulz L, Ackley C, Fenske N (2010) Adsorption of tetracycline on kaolinite with ph-dependent surface charges. J Colloid Interface Sci 351(1):254–260

    Article  CAS  Google Scholar 

  • Li G, Zhang D, Wang M, Huang J, Huang L (2013) Preparation of activated carbons from Iris tectorum employing ferric nitrate as dopant for removal of tetracycline from aqueous solutions. Ecotoxicol Environ Saf 98(dec.1):273–282

    Article  CAS  Google Scholar 

  • Li H, Dong X, Silva EB, Oliveira LM, Chen Y, Ma LQ (2017) Mechanisms of metal sorption by biochars: biochar characteristics and modifications. J Chemosphere 178:466–478

    Article  CAS  Google Scholar 

  • Liu S, Xu WH, Liu YG, Tan XF, Zeng GM, Li X, Liang J, Zhou Z, Yan ZL, Cai XX (2017) Facile synthesis of Cu(II) impregnated biochar with enhanced adsorption activity for the removal of doxycycline hydrochloride from water. Sci Total Environ 592:546–553

    Article  CAS  Google Scholar 

  • Lofrano G, Libralato G, Casaburi A, Siciliano A, Iannece P, Guida M, Pucci L, Dentice EF, Carotenuto M (2018) Municipal wastewater spiramycin removal by conventional treatments and heterogeneous photocatalysis. Sci Total Environ 624:461–469

    Article  CAS  Google Scholar 

  • Lingeswarran M, Farook A, Abdul RM, Eng-Poh Ng (2014) The synthesis and characterization of high purity mixed microporous/mesoporous activated carbon from rice husk using chemical activation with NaOH and KOH. Microporous and Mesoporous Mater. https://doi.org/10.1016/j.micromeso.2014.06.020

  • Peng W, Xie Z, Cheng G, Shi L, Zhang Y (2015) Amino-functionalized adsorbent prepared by means of cu(ii) imprinted method and its selective removal of copper from aqueous solutions. J Hazard Mater 294(aug.30):9–16

    Article  CAS  Google Scholar 

  • Prakash O, Singh SK, Singh B, Singh RK (2013) Investigation of coordination properties of isolated adenine to copper metal: a systematic spectroscopic and dft study. Spectrochimica Acta Part A Molecular and Biomolecular Spectroscopy 112C:410–416

    Article  Google Scholar 

  • Siddiqui H, Qureshi MS, Haque FZ (2016) Effect of copper precursor salts: facile and sustainable synthesis of controlled shaped copper oxide nanoparticles. Optik - Int J Light Electron Optics:4726–4730

  • Tan X, Liu Y, Zeng G, Wang X, Hu X, Gu Y et al (2015) Application of biochar for the removal of pollutants from aqueous solutions. Chemosphere 125(apr.):70–85

    Article  CAS  Google Scholar 

  • Tan X, Liu S, Liu Y, Gu Y, Zeng G, Cai X, Yan ZL, Yang C, Hu X, Chen B (2016) One-pot synthesis of carbon supported calcined-mg/al layered double hydroxides for antibiotic removal by slow pyrolysis of biomass waste. Sci Rep 6(1):39691

    Article  CAS  Google Scholar 

  • Tang L, Yu J, Pang Y, Zeng G, Deng Y, Wang J, Feng H (2018) Sustainable efficient adsorbent: Alkali-acid modified magnetic biochar derived from sewage sludge for aqueous organic contaminant removal. Chem Eng J 336:160–169. https://doi.org/10.1016/j.cej.2017.11.048

    Article  CAS  Google Scholar 

  • Tong Z, Wang T, Ma R, Wen L, Feng C, Sun W (2018) Influences of isolated fractions of natural organic matter on adsorption of cu(ii) by titanate nanotubes. Sci Total Environ 650:1412–1418

    Google Scholar 

  • Van Stempvoort JWR, Grabuski J et al (2013) An artificial sweetener and pharmaceutical compounds as co-tracers of urban wastewater in groundwater. Science of the Total Environment 461-462(sep.1):348–359. https://doi.org/10.1016/j.scitotenv.2013.05.001

    Article  CAS  Google Scholar 

  • Wan X, Gao M, Ye M, Wang YK, Xu H, Wang M, Wang XH (2017) Formation, characteristics and microbial community of aerobic granular sludge in the presence of sulfadiazine at environmentally relevant concentrations. Bioresour Technol 250:486–494

    Article  Google Scholar 

  • Wang B, Li C, Liang H (2013) Bioleaching of heavy metal from woody biochar using acidithiobacillus ferrooxidans and activation for adsorption. Bioresour Technol 146:803–806

    Article  CAS  Google Scholar 

  • Wang Z, Han L, Sun K, Jin J, Ro KS, Libra JA et al (2016) Sorption of four hydrophobic organic contaminants by biochars derived from maize straw, wood dust and swine manure at different pyrolytic temperatures. Chemosphere 144(FEB):285–291

    Article  CAS  Google Scholar 

  • Wang B, Jiang Y-s, Li F-y, Yang D-y (2017) Preparation of biochar by simultaneous carbonization, magnetization and activation for norfloxacin removal in water. Bioresour Technol 233(Complete):159–165

    Article  CAS  Google Scholar 

  • Weisheng G, Xu W, Pan J et al (2012) Synthesis of magnetic halloysite composites for the effective removal of tetracycline hydrochloride from aqueous solutions. Adsorpt Sci Technol 7:579–591. https://doi.org/10.1260/0263-6174.30.7.579

    Article  Google Scholar 

  • Xiangdong Z, Yuchen L, Feng Q et al (2014) Preparation of magnetic porous carbon from waste hydrochar by simultaneous activation and magnetization for tetracycline removal. Bioresour Technol 154(1):209–214

    Google Scholar 

  • Xu X, Cao X, Zhao L (2013) Comparison of rice husk- and dairy manure-derived biochars for simultaneously removing heavy metals from aqueous solutions: role of mineral components in biochars. Chemosphere 92(8):955–961

    Article  CAS  Google Scholar 

  • Yan L, Liu Y, Zhang Y, Liu S, Wang C, Chen W, Liu C, Chen Z, Zhang Y (2020) ZnCl2 modified biochar derived from aerobic granular sludge for developed microporosity and enhanced adsorption to tetracycline. Bioresour Technol 297:122381. https://doi.org/10.1016/j.biortech.2019.122381

    Article  CAS  Google Scholar 

  • Yang GX, Jiang H (2014) Amino modification of biochar for enhanced adsorption of copper ions from synthetic wastewater. Water Res 48(jan.1):396–405

    Article  CAS  Google Scholar 

  • Yang Z, Jia S, Zhang T, Zhuo N, Dong Y, Yang W, Wang Y (2015) How heavy metals impact on flocculation of combined pollution of heavy metals–antibiotics: a comparative study. Separation and Purification Technology:149

  • Yang X, Xu G, Yu H, Zhang Z (2016) Preparation of ferric-activated sludge-based adsorbent from biological sludge for tetracycline removal. Bioresour Technol 211:566–573

    Article  CAS  Google Scholar 

  • Yu JY, Li W, Chen X (2012) Highly enhanced electrocatalytic oxidation of glucose on Cu(OH)2/CuO nanotube arrays modified copper electrode. J Solid State Electrochem 16(9):2877–2881

    Article  Google Scholar 

  • Yu F, Li Y, Han S, Ma J (2016) Adsorptive removal of antibiotics from aqueous solution using carbon materials. Chemosphere 153:365–385. https://doi.org/10.1016/j.chemosphere.2016.03.083

    Article  CAS  Google Scholar 

  • Zawani Z, Luqman CA, Choong T (2009) Equilibrium, kinetics and thermodynamic studies: adsorption of remazol black 5 on the palm kernel shell activated carbon (pks-ac). Eur J Sci Res 37(1):67–76

    Google Scholar 

  • Zhang G, Shi L, Zhang Y, Wei D, Yan T, Wei Q, du B (2015a) Aerobic granular sludge-derived activated carbon: mineral acid modification and superior dye adsorption capacity. RSC Adv 5(32):25279–25286

    Article  CAS  Google Scholar 

  • Zhang QQ, Ying GG, Pan CG, Liu YS, Zhao JLJES, Technology (2015b) Comprehensive evaluation of antibiotics emission and fate in the river basins of China: source analysis, multimedia modeling, and linkage to bacterial resistance. Environ Sci Technol 49(11):6772–6782

    Article  CAS  Google Scholar 

  • Zhang Z, Pan Z, Guo Y, Wong PK, Zhou X, Bai R (2020) In-situ growth of all-solid Z-scheme heterojunction photocatalyst of Bi7O9I3/g-C3N4 and high efficient degradation of antibiotic under visible light. Appl Catal B Environ:261. https://doi.org/10.1016/j.apcatb.2019.118212

  • Zhao Y, Gu X, Gao S, Geng J, Wang X (2012) Adsorption of tetracycline (TC) onto montmorillonite: cations and humic acid effects. Geoderma 183-184(none):12–18

    Article  CAS  Google Scholar 

  • Zhou Y, Liu X, Xiang Y, Wang P, Zhang J, Zhang F et al (2017) Modification of biochar derived from sawdust and its application in removal of tetracycline and copper from aqueous solution: adsorption mechanism and modelling. Bioresour Technol:266–273

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Acknowledgements

We thank the Lanzhou Branch, Institute of Chemical Physics, Chinese Academy of Sciences, for finishing the SEM, XPS, and BET representation of the prepared materials.

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The datasets generated or analyzed during the current study are not publicly available due [REASON WHY DATA ARE NOT PUBLIC] but are available from the corresponding author on reasonable request.

Funding

This study was supported by the National Natural Science Foundation of China (21667017, 22166023).

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XZ was responsible for cultivating granular sludge, and was a major contributor in writing the manuscript. HW was responsible for the preparation and analysis of biochar. GZ, WP, and YX were responsible for the section of the adsorption experiment. All authors read and approved the final manuscript.

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Correspondence to Xia Zhao.

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Zhao, X., Wang, H., Zhang, G. et al. Characteristics of Cu(II)-modified aerobic granular sludge biocarbon in removal of doxycycline hydroxide. Environ Sci Pollut Res 29, 14019–14035 (2022). https://doi.org/10.1007/s11356-021-16547-x

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