Skip to main content
Log in

Adsorption Characteristics and Mechanisms of Oxytetracycline on Nano Biochar: Effects of Environmental Conditions and Particle Aggregation

  • Published:
Water, Air, & Soil Pollution Aims and scope Submit manuscript

Abstract

Physical disintegration of macro biochars in natural environments produces nano biochars, thus affecting environmental processes (e.g., adsorption, migration) of antibiotic contaminants. However, knowledge about the relationships between adsorption behaviors of antibiotics and unique physicochemical colloidal properties of nano biochar are relatively limited. In this study, a nano biochar (NSD700) was prepared from sawdust-derived biochar (SD700) by a combination method of ball milling, sonication, and centrifugation to contrastively investigate their adsorption for oxytetracycline (OTC). NSD700 had similar chemical structure properties of carbon fraction with SD700, whereas NSD700 possessed greater surface area and porosity. The maximal sorption capacity of OTC on NSD700 was 30.7 mg/g, ~3 times greater than that of SD700 (10.4 mg/g), primarily benefiting from more exposed surfaces and pores. OTC adsorption on NSD700 was inhibited under acidic and alkaline condition, and the inhibiting effect was more significant in comparison with that on SD700. OTC sorption onto NSD700 gradually decreased with increasing concentration of Na+, but was not observed for SD700. Aggregation kinetic of NSD700 varying with Na+ concentration demonstrated that the inhibiting effect might be affiliated with the destabilization and aggregation of NSD700, which could obstruct adsorption sites. This study provided insights for antibiotic adsorption characteristics on nano biochar and will help understanding the process and fate of antibiotics in the biochar-remediated environment.

Graphical Abstract

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6

Similar content being viewed by others

Data Availability

All relevant data are within the paper.

Abbreviations

OTC:

Oxytetracycline

SD700:

Sawdust-derived biochar

NSD700:

Nano biochar

NaCl:

Sodium chloride

NaOH:

Sodium hydroxide

HCl:

Hydroxide acid

SEM:

Scanning electron microscope

TEM:

Transmission electron microscope

AFM:

Atomic force microscope

XRD:

X-ray diffractometer

FTIR:

Fourier transform infrared spectroscopy

DXR3:

Raman spectroscopy

DR:

Dubinin-Radushkevich

BET:

Brunauere-Emmette-Teller

BJH:

Berret-Joyner-Halenda

HPLC:

High-performance liquid chromatography

References

  • Annamalai, S., & Shin, W. (2022). Efficient degradation of trimethoprim with ball-milled nitrogen-doped biochar catalyst via persulfate activation. Chemical Engineering Journal, 440, 135815.

    CAS  Google Scholar 

  • Bai, B., Nie, Q., Zhang, Y., et al. (2021). Cotransport of heavy metals and SiO2 particles at different temperatures by seepage. Journal of Hydrology, 597, 125771.

    CAS  Google Scholar 

  • Bai, B., Rao, D., Chang, T., et al. (2019). A nonlinear attachment-detachment model with adsorption hysteresis for suspension-colloidal transport in porous media. Journal of Hydrology, 578, 124080.

    CAS  Google Scholar 

  • Ben, Y., Hu, M., Zhang, X., et al. (2020). Efficient detection and assessment of human exposure to trace antibiotic residues in drinking water. Water Research, 175, 115699.

    CAS  Google Scholar 

  • Bian, S., Xu, S., Yin, Z., et al. (2021). An efficient strategy for enhancing the adsorption capabilities of biochar via sequential KMnO4-promoted oxidative pyrolysis and H2O2 oxidation. Sustainability, 13(5), 2641.

    CAS  Google Scholar 

  • Cao, Y., Xiao, W., Shen, G., et al. (2019). Carbonization and ball milling on the enhancement of Pb(II) adsorption by wheat straw: Competitive effects of ion exchange and precipitation. Bioresource Technology, 273, 70–76.

    CAS  Google Scholar 

  • Chen, Y., Lin, Y., Ho, S., et al. (2018). Highly efficient adsorption of dyes by biochar derived from pigments-extracted macroalgae pyrolyzed at different temperature. Bioresource Technology, 259, 104–110.

    CAS  Google Scholar 

  • Fan, R., Chen, C., Lin, J., et al. (2019). Adsorption characteristics of ammonium ion onto hydrous biochars in dilute aqueous solutions. Bioresource Technology, 272, 465–472.

    CAS  Google Scholar 

  • Gámiz, B., Velarde, P., Spokas, K., et al. (2019). Changes in sorption and bioavailability of herbicides in soil amended with fresh and aged biochar. Geoderma, 337, 341–349.

    Google Scholar 

  • Guenay, A., Arslankaya, E., & Tosun, I. (2007). Lead removal from aqueous solution by natural and pretreated clinoptilolite: Adsorption equilibrium and kinetics. Journal of Hazardous Materials, 146(1-2), 362–371.

    CAS  Google Scholar 

  • Hou, J., Wang, C., Mao, D., et al. (2016). The occurrence and fate of tetracyclines in two pharmaceutical wastewater treatment plants of Northern China. Environmental Science and Pollution Research, 23(2), 1722–1731.

    CAS  Google Scholar 

  • Huang, J., Zimmerman, A., Chen, H., et al. (2020). Ball milled biochar effectively removes sulfamethoxazole and sulfapyridine antibiotics from water and wastewater. Environmental Pollution, 258, 113809.

    CAS  Google Scholar 

  • Jia, S., Zhang, X., Miao, Y., et al. (2017). Fate of antibiotic resistance genes and their associations with bacterial community in livestock breeding wastewater and its receiving river water. Water Research, 124, 259–268.

    CAS  Google Scholar 

  • Kearns, J., Wellborn, L., Summers, R., et al. (2014). 2,4-D adsorption to biochars: effect of preparation conditions on equilibrium adsorption capacity and comparison with commercial activated carbon literature data. Water Research, 62, 20–28.

    CAS  Google Scholar 

  • Khadem, A., Raiesi, F., Besharati, H., et al. (2021). The effects of biochar on soil nutrients status, microbial activity and carbon sequestration potential in two calcareous soils. Biochar, 3(1), 105–116.

    CAS  Google Scholar 

  • Kumar, M., Xiong, X., Wan, Z., et al. (2020). Ball milling as a mechanochemical technology for fabrication of novel biochar nanomaterials. Bioresource Technology, 312, 123613.

    CAS  Google Scholar 

  • Larsson, D., & Flach, C. (2022). Antibiotic resistance in the environment. Nature Reviews Microbiology, 20(5), 257–269.

    CAS  Google Scholar 

  • Li, R., Zhang, Y., Deng, H., et al. (2020). Removing tetracycline and Hg(II) with ball-milled magnetic nanobiochar and its potential on polluted irrigation water reclamation. Journal of Hazardous Materials, 384, 10.

    Google Scholar 

  • Li, X., Jia, Y., Zhou, M., et al. (2020). High-efficiency degradation of organic pollutants with Fe, N co-doped biochar catalysts via persulfate activation. Journal of Hazardous Materials, 397, 122764.

    CAS  Google Scholar 

  • Lian, F., & Xing, B. (2017). Black carbon (biochar) in water/soil environments: Molecular structure, sorption, stability, and potential risk. Environmental Science & Technology, 51(23), 13517–13532.

    CAS  Google Scholar 

  • Lian, F., Yu, W., Wang, Z., et al. (2018). New insights into black carbon nanoparticle-induced dispersibility of goethite colloids and configuration-dependent sorption for phenanthrene. Environmental Science & Technology, 53(2), 661–670.

    Google Scholar 

  • Lian, F., Yu, W., Zhou, Q., et al. (2020). Size matters: Nano-biochar triggers decomposition and transformation inhibition of antibiotic resistance genes in aqueous. Environmental Science & Technology, 54(14), 8821–8829.

    CAS  Google Scholar 

  • Liu, G., Chen, L., Jiang, Z., et al. (2017). Aging impacts of low molecular weight organic acids (LMWOAs) on furfural production residue-derived biochars: Porosity, functional properties, and inorganic minerals. Science of the Total Environment, 607-608, 1428–1436.

    CAS  Google Scholar 

  • Liu, G., Pan, M., Song, J., et al. (2022). Investigating the effects of biochar colloids and nanoparticles on cucumber early seedlings. Science of the Total Environment, 804, 150233.

    CAS  Google Scholar 

  • Liu, G., Zheng, H., Jiang, Z., et al. (2018). Formation and physicochemical characteristics of nano biochar: Insight into chemical and colloidal stability. Environmental Science and Technology, 52(18), 10369–10379.

    CAS  Google Scholar 

  • Lyu, H., Gao, B., He, F., et al. (2018). Effects of ball milling on the physicochemical and sorptive properties of biochar: Experimental observations and governing mechanisms. Environmental Pollution, 233, 54–63.

    CAS  Google Scholar 

  • Lyu, J., Yang, L., Zhang, L., et al. (2020). Antibiotics in soil and water in China–A systematic review and source analysis. Environmental Pollution, 266, 115147.

    Google Scholar 

  • Major, J. (2010). Guidelines on practical aspects of biochar application to field soil in various soil management systems. International Biochar Initiative, 1, 6–8.

    Google Scholar 

  • Nazari, S., Asgari, E., Sheikhmohammadi, A., et al. (2023). Visible-light-driven photocatalytic activity of WO3/ZIF-67 S-scheme heterojunction for upgrading degradation of oxytetracycline. Journal of Environmental Chemical Engineering, 11(5), 11039.

  • Ngigi, A., Ok, Y., & Thiele-Bruhn, S. (2019). Biochar-mediated sorption of antibiotics in pig manure. Journal of Hazardous Materials, 364, 663–670.

    CAS  Google Scholar 

  • Qi, W., Long, J., Feng, C., et al. (2019). Fe3+ enhanced degradation of oxytetracycline in water by pseudomonas. Water Research, 160, 361–370.

    CAS  Google Scholar 

  • Qu, X., Fu, H., Mao, J., et al. (2016). Chemical and structural properties of dissolved black carbon released from biochars. Carbon, 96, 759–767.

    CAS  Google Scholar 

  • Ramanayaka, S., Vithanage, M., Alessi, D., et al. (2020). Nanobiochar: Production, properties, and multifunctional applications. Environmental Science: Nano, 7(11), 3279–3302.

    CAS  Google Scholar 

  • Ren, X., Wang, F., Zhang, P., et al. (2018). Aging effect of minerals on biochar properties and sorption capacities for atrazine and phenanthrene. Chemosphere, 206, 51–58.

    CAS  Google Scholar 

  • Shen, Q., Wang, Z., Yu, Q., et al. (2020). Removal of tetracycline from an aqueous solution using manganese dioxide modified biochar derived from Chinese herbal medicine residues. Environmental Research, 183, 109195.

    CAS  Google Scholar 

  • Song, B., Chen, M., Zhao, L., et al. (2019). Physicochemical property and colloidal stability of micron- and nano-particle biochar derived from a variety of feedstock sources. Science of the Total Environment, 661, 685–695.

    CAS  Google Scholar 

  • Song, J., Lu, L., Wang, J., et al. (2023). Highly efficient nanocomposite of Y2O3@biochar for oxytetracycline removal from solution: Adsorption characteristics and mechanisms. Bioresource Technology, 385, 129380.

    CAS  Google Scholar 

  • Sorrenti, G., Masiello, C., Dugan, B., et al. (2016). Biochar physico-chemical properties as affected by environmental exposure. Science of the Total Environment, 563-564, 237–246.

    CAS  Google Scholar 

  • Tang, J., Ma, Y., Zeng, C., et al. (2023). Fe-Al bimetallic oxides functionalized-biochar via ball milling for enhanced adsorption of tetracycline in water. Bioresource Technology, 369, 128385.

    CAS  Google Scholar 

  • Tang, L., Zhou, S., Li, F., et al. (2022). Ozone micronano-bubble-enhanced selective degradation of oxytetracycline from production wastewater: The overlooked singlet oxygen oxidation. Environmental Science and Technology.

  • Tang, W., Jing, F., Laurent, Z., et al. (2021). High-temperature and freeze-thaw aged biochar impacts on sulfonamide sorption and mobility in soil. Chemosphere, 276, 130106.

    CAS  Google Scholar 

  • Wang, B., Gao, B., Zimmerman, A., et al. (2018). Novel biochar-impregnated calcium alginate beads with improved water holding and nutrient retention properties. Journal of Environmental Management, 209, 105–111.

    Google Scholar 

  • Wang, H., Lou, X., Hu, Q., et al. (2021). Adsorption of antibiotics from water by using Chinese herbal medicine residues derived biochar: Preparation and properties studies. Journal of Molecular Liquids, 325, 114967.

    CAS  Google Scholar 

  • Wang, L., O’Connor, D., Rinklebe, J., et al. (2020). Biochar aging: Mechanisms, physicochemical changes, assessment, and implications for field applications. Environmental Science & Technology, 54(23), 14797–14814.

    CAS  Google Scholar 

  • Wang, Y., Zhang, W., Shang, J., et al. (2019). Chemical aging changed aggregation kinetics and transport of biochar colloids. Environmental Science & Technology, 53(14), 8136–8146.

    CAS  Google Scholar 

  • Wang, Z., Chen, Q., Zhang, J., et al. (2019). Characterization and source identification of tetracycline antibiotics in the drinking water sources of the lower Yangtze River. Journal of Environmental Management, 244, 13–22.

    Google Scholar 

  • Wu, Z., Wang, M., Bai, Y., et al. (2023). Upcycling of nickel iron slags to hierarchical self-assembled flower-like photocatalysts for highly efficient degradation of high-concentration tetracycline. Chemical Engineering Journal, 464, 142532.

    CAS  Google Scholar 

  • Xiang, W., Wan, Y., Zhang, X., et al. (2020). Adsorption of tetracycline hydrochloride onto ball-milled biochar: Governing factors and mechanisms. Chemosphere, 255, 127057.

    CAS  Google Scholar 

  • Xu, D., Gao, Y., Lin, Z., et al. (2019). Application of biochar derived from pyrolysis of waste fiberboard on tetracycline adsorption in aqueous solution. Frontiers in Chemistry, 7, 943.

    CAS  Google Scholar 

  • Xu, X., Zheng, Y., Gao, B., et al. (2019). N-doped biochar synthesized by a facile ball-milling method for enhanced sorption of CO2 and reactive red. Chemical Engineering Journal, 368, 564–572.

    CAS  Google Scholar 

  • Xue, C., Wu, J., Wang, K., et al. (2021). Effects of different types of biochar on the properties and reactivity of nano zero-valent iron in soil remediation. Frontiers of Environmental Science & Engineering, 15(5), 101.

    CAS  Google Scholar 

  • Yang, Y., Duan, P., Schmidt-Rohr, K., et al. (2021). Physicochemical changes in biomass chars by thermal oxidation or ambient weathering and their impacts on sorption of a hydrophobic and a cationic compound. Environmental Science & Technology, 55(19), 13072–13081.

    CAS  Google Scholar 

  • Yu, F., Ma, J., & Han, S. (2014). Adsorption of tetracycline from aqueous solutions onto multi-walled carbon nanotubes with different oxygen contents. Scientific Reports, 4, 5326.

    CAS  Google Scholar 

  • Zhang, D., He, Q., Hu, X., et al. (2021). Enhanced adsorption for the removal of tetracycline hydrochloride (TC) using ball-milled biochar derived from crayfish shell. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 615, 126254.

    CAS  Google Scholar 

  • Zhang, Q., Wang, J., Lyu, H., et al. (2019). Ball-milled biochar for galaxolide removal: Sorption performance and governing mechanisms. Science of the Total Environment, 659, 1537–1545.

    CAS  Google Scholar 

  • Zhang, Y., Zhang, J., Chen, K., et al. (2023). Engineering banana-peel-derived biochar for the rapid adsorption of tetracycline based on double chemical activation. Resources, Conservation and Recycling, 190, 106821.

    CAS  Google Scholar 

  • Zhang, Y., Zheng, Y., Yang, Y., et al. (2021). Mechanisms and adsorption capacities of hydrogen peroxide modified ball milled biochar for the removal of methylene blue from aqueous solutions. Bioresource Technology, 337, 125432.

    CAS  Google Scholar 

  • Zhao, Z., Wang, B., Zhang, X., et al. (2022). Release characteristics of phosphate from ball-milled biochar and its potential effects on plant growth. Science of The Total Environment, 821, 153256.

    CAS  Google Scholar 

  • Zheng, H., Zhang, Q., Liu, G., et al. (2019). Characteristics and mechanisms of chlorpyrifos and chlorpyrifos-methyl adsorption onto biochars: Influence of deashing and low molecular weight organic acid (LMWOA) aging and co-existence. Science of the Total Environment, 657, 953–962.

    CAS  Google Scholar 

Download references

Acknowledgements

We thank Natural Science Foundation of Shandong Province (ZR2020MD112), National Natural Science Foundation of China (52170135, 52070107), and Research Foundation for Talented Scholars of Qingdao Agricultural University (6651119010) for conducting the experiments.

Author information

Authors and Affiliations

Authors

Contributions

All authors contributed to the study conception and design. Wenqiang Jia contributed to the conception of the study and wrote the manuscript. Investigation, data curation, and formal analysis were performed by Wenqiang Jia and Xiangrui Pan. Data curation and formal analysis were performed by Jiaying Song, Jian Wang, and Weikai Sun. Supervision and funding acquisition were performed by Yanjun Xin. Supervision and investigation were performed by Qinghua Yan and Chengzhi Zhou. Conceptualization, writing—review and editing, resources, supervision, and funding acquisition were performed by Hao Zheng and Guocheng Liu. All authors read and approved the final manuscript.

Corresponding authors

Correspondence to Hao Zheng or Guocheng Liu.

Ethics declarations

Ethics Approval

Not applicable.

Consent to Participate

Not applicable.

Consent for Publication

All authors consented when it was submitted.

Competing Interests

The authors declare no competing interests.

Additional information

Publisher’s Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Core Ideas

• OTC adsorption on macro and nano biochar was investigated contrastively

• Greater surface area and more pores of nano biochar favor OTC adsorption

• Aggregation of nano biochar due to coexisting cation may shield adsorption sites

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Jia, W., Pan, X., Song, J. et al. Adsorption Characteristics and Mechanisms of Oxytetracycline on Nano Biochar: Effects of Environmental Conditions and Particle Aggregation. Water Air Soil Pollut 234, 616 (2023). https://doi.org/10.1007/s11270-023-06633-w

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s11270-023-06633-w

Keywords

Navigation