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Preparation of ZIF-67/C3N4 composite material and adsorption of tetracycline hydrochloride

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Abstract

In recent years, wastewater treatment to remove tetracycline hydrochloride (TCH) has received much attention in water treatment problems. ZIF-67/C3N4 composite adsorbent, a nanosheet structured material stacked with MOFs, was prepared by in situ growth method, which has high adsorption activity for tetracycline hydrochloride in wastewater. Comparing the effect of monomeric and composite adsorbents, Z6C2 had the best adsorption effect (206 mg·g−1), which was 77.6% higher than that of ZIF-67 (116 mg·g−1) and 10.8 times higher than that of C3N4 (19 mg·g−1). The structure of ZIF-67 stacked on C3N4 nanosheets has an excellent specific surface area and number of active sites, as well as π-π interactions, electrostatic interactions, and hydrogen bonding interactions between the adsorbent and TCH, which combine to enhance the adsorption performance. The adsorption process is accompanied by a combination of chemisorption, mass transport, and internal diffusion rate-limiting. It was shown that the adsorption process is favorable for monolayer adsorption as well as a heat absorption reaction that proceeds spontaneously. The adsorbent exhibits good stability and adsorption capacity, which may be suitable for efficient and low-cost water purification.

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The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request. All data generated or analyzed during this study are included in this published article.

References

  • Ahmad F, Zhu D, Sun J (2021) Environmental fate of tetracycline antibiotics: degradation pathway mechanisms, challenges, and perspectives. Environ Sci Eur 33(1):64

    Google Scholar 

  • Bacanlı M, Başaran N (2019) Importance of antibiotic residues in animal food. Food Chem Toxicol 125:462–466

    Google Scholar 

  • Bangari RS, Sinha N (2019) Adsorption of tetracycline, ofloxacin and cephalexin antibiotics on boron nitride nanosheets from aqueous solution. J Mol Liq 293:111376

    CAS  Google Scholar 

  • Barrio Hermida J, Volokh M, Shalom M (2020) Polymeric carbon nitrides and related metal-free materials for energy and environmental applications. J Mater Chem A 8:11075–11116

    Google Scholar 

  • Cai X, He J, Chen L, Chen K, Li Y, Zhang K, Jin Z, Liu J, Wang C, Wang X, Kong L, Liu J (2017) A 2D-g-C3N4 nanosheet as an eco-friendly adsorbent for various environmental pollutants in water. Chemosphere 171:192–201

    CAS  Google Scholar 

  • Chang Q, Ali A, Su J, Wen Q, Bai Y, Gao Z (2021) Simultaneous removal of nitrate, manganese, and tetracycline by Zoogloea sp. MFQ7: Adsorption mechanism of tetracycline by biological precipitation. Bioresour Technol 340:125690

    CAS  Google Scholar 

  • Chen W-Q, Li L-Y, Li L, Qiu W-H, Tang L, Xu L, Xu K-J, Wu M-H (2019) MoS2/ZIF-8 hybrid materials for environmental catalysis: solar-driven antibiotic-degradation engineering. Engineering 5(4):755–767

    CAS  Google Scholar 

  • Chen B, Li Y, Li M, Cui M, Xu W, Li L, Sun Y, Wang M, Zhang Y, Chen K (2021) Rapid adsorption of tetracycline in aqueous solution by using MOF-525/graphene oxide composite. Microporous Mesoporous Mater 328:111457

    CAS  Google Scholar 

  • Danon A, Stair P, Weitz E (2011) FTIR study of CO2 adsorption on amine-grafted SBA-15: Elucidation of adsorbed species. J Phys Chem C 115(23):11540–11549

    CAS  Google Scholar 

  • Dao X, Hao H, Bi J, Sun S, Huang X (2022) Surface complexation enhanced adsorption of tetracycline by ALK-MXene. Ind Eng Chem Res 61(17):6028–6036

    CAS  Google Scholar 

  • Fu J, Yu J, Jiang C, Cheng B (2017) g-C3N4-based heterostructured photocatalysts. Adv Energy Mater 8:1701503

    Google Scholar 

  • Hou C, Liu H, Mohammad FB (2021) Preparation of ordered mesoporous F-H2Ti3O7 nanosheets using orthorhombic HTiOF3 as a precursor and their highly efficient degradation of tetracycline hydrochloride under simulated sunlight. J Solid State Chem 300:122288

    CAS  Google Scholar 

  • Howarth AJ, Peters AW, Vermeulen NA, Wang TC, Hupp JT, Farha OK (2017) Best practices for the synthesis, activation, and characterization of metal–organic frameworks. Chem Mater 29(1):26–39

    CAS  Google Scholar 

  • Jadhav H, Bandal H, Ramakrishna S, Kim H (2022) Critical review, recent updates on Zeolitic Imidazolate Framework-67 (ZIF-67) and its derivatives for electrochemical water splitting. Adv Mater 34:2107072

    CAS  Google Scholar 

  • Jafari Ozumchelouei E, Hamidian AH, Zhang Y, Yang M (2019) Physico-chemical properties of antibiotics: a review with an emphasis on detection in the aquatic environment. Water Environ Res 92:177–188

    Google Scholar 

  • Jh A, Yx A, Wei WB, Bo HA, Zw A, Xin YC, Yu WD, Ly A (2020) Ce(III) nanocomposites by partial thermal decomposition of Ce-MOF for effective phosphate adsorption in a wide pH range. Chem Eng J 379:122431

    Google Scholar 

  • Jin J, Yang Z, Xiong W, Zhou Y, Xu R, Zhang Y, Cao J, Li X, Zhou C (2019) Cu and Co nanoparticles co-doped MIL-101 as a novel adsorbent for efficient removal of tetracycline from aqueous solutions. Sci Total Environ 650:408–418

    CAS  Google Scholar 

  • Kc D, Vattikuti SV, Tvm S, Yoo K, Nagajyothi PC, Shim J (2020) Hydrogen production and photocatalytic activity of g-C3N4/Co-MOF (ZIF-67) nanocomposite under visible light irradiation. Appl Organomet Chem 34(3):e4376

    Google Scholar 

  • Kong Y, Zhuang Y, Han K, Shi B (2020) Enhanced tetracycline adsorption using alginate-graphene-ZIF67 aerogel. Colloids Surf, A 588:124360

    CAS  Google Scholar 

  • Lee P-Y, Lin L-Y, Hsu IJ, Chan C-Y, Lee J-F, Sheu H-S (2021) Facile synthesis of perovskite ZIF67 derivative using ammonia fluoride and comparison with post-treated ZIF67 derivatives on energy storage ability. Electrochim Acta 389:138680

    CAS  Google Scholar 

  • Li Y, Zhou K, He M, Yao J (2016) Synthesis of ZIF-8 and ZIF-67 using mixed-base and their dye adsorption. Microporous Mesoporous Mater 234:287–292

    CAS  Google Scholar 

  • Li Y, Yan X, Hu X, Feng R, Zhou M (2019) Trace pyrolyzed ZIF-67 loaded activated carbon pellets for enhanced adsorption and catalytic degradation of Rhodamine B in water. Chem Eng J 375:122003

    CAS  Google Scholar 

  • Li B, Igawa K, Chai J, Chen Y, Wang Y, Fam DW, Tham NN, An T, Konno T, Sng A, Liu Z, Zhang H, Zong Y (2020) String of pyrolyzed ZIF-67 particles on carbon fibers for high-performance electrocatalysis. Energy Storage Mater 25:137–144

    Google Scholar 

  • Liao R, Li M, Li W, Lin X, Liu D, Wang L (2018) Efficient absorption of ibuprofen in aqueous solution using eco-friendly C3N4/soot composite. J Mater Sci 53(8):5929–5941

    CAS  Google Scholar 

  • Liu H, Yu D, Sun T, Du H, Jiang W, Muhammad Y, Huang L (2019a) Fabrication of surface alkalinized g-C3N4 and TiO2 composite for the synergistic adsorption-photocatalytic degradation of methylene blue. Appl Surf Sci 473:855–863

    CAS  Google Scholar 

  • Liu J, Zhou B, Zhang H, Ma J, Mu B, Zhang W (2019b) A novel Biochar modified by Chitosan-Fe/S for tetracycline adsorption and studies on site energy distribution. Biores Technol 294:122152

    CAS  Google Scholar 

  • Liu M, Zhang D, Han J, Liu C, Ding Y, Wang Z, Wang A (2020) Adsorption enhanced photocatalytic degradation sulfadiazine antibiotic using porous carbon nitride nanosheets with carbon vacancies. Chem Eng J 382:123017

    CAS  Google Scholar 

  • Liu J, Lin H, Dong Y, He Y, Liu W, Shi Y (2021) The effective adsorption of tetracycline onto MoS2@Zeolite-5: adsorption behavior and interfacial mechanism. J Environ Chem Eng 9(5):105912

    CAS  Google Scholar 

  • Liu B, Zhang L, Yao Q, Chen Q, Zhao X (2022) Magnetic porous carbons derived from metal-organic frameworks for effective adsorption of tetracycline. J Solid State Chem 316:123603

    CAS  Google Scholar 

  • Lv P, Duan F, Sheng J, Lu S, Du M, Chen M (2021) The 2D/2D p–n heterojunction of ZnCoMOF/g-C3N4 with enhanced photocatalytic hydrogen evolution under visible light irradiation. Appl Organomet Chem 35:e6124

    CAS  Google Scholar 

  • Masoumi S, Farshchi Tabrizi F, Sardarian AR (2020) Efficient tetracycline hydrochloride removal by encapsulated phosphotungstic acid (PTA) in MIL–53 (Fe): Optimizing the content of PTA and recycling study. J Environ Chem Eng 8(1):103601

    CAS  Google Scholar 

  • Muelas-Ramos V, Sampaio MJ, Silva CG, Bedia J, Rodriguez JJ, Faria JL, Belver C (2021) Degradation of diclofenac in water under LED irradiation using combined g-C3N4/NH2-MIL-125 photocatalysts. J Hazard Mater 416:126199

    CAS  Google Scholar 

  • Panneri S, Thomas M, Ganguly P, Nair B, Peer A, Warrier K, Hareesh US (2017) C3N4 Anchored ZIF 8 composites: photo-regenerable, high capacity sorbents as adsorptive photocatalysts for the effective removal of tetracycline from water. Catal Sci Technol 7:2118–2128

    CAS  Google Scholar 

  • Qian X, Wu H, Ma S, H. zhu and G. zhu, (2016) Controlled synthesis of highly stable zeolitic imidazolate framework-67 dodecahedra and their use towards the templated formation of hollow Co3O4 catalyst for CO oxidation. RSC Adv 6:6915–6920

    Google Scholar 

  • Qiao D, Li Z, Duan J, He X (2020) Adsorption and photocatalytic degradation mechanism of magnetic graphene oxide/ZnO nanocomposites for tetracycline contaminants. Chem Eng J 400:125952

    CAS  Google Scholar 

  • Qin Q, Wu X, Chen L, Jiang Z, Xu Y (2018) Simultaneous removal of tetracycline and Cu(II) by adsorption and coadsorption using oxidized activated carbon. RSC Adv 8:1744–1752

    CAS  Google Scholar 

  • Ran G, Yang J, Xing Y, Zhang Y, Tang X, Hu Q, Huang K, Zou Z, Yu H, Xiong X (2023) A novel Co3Mo3N self-embedded in porous carbon nanocomposite derived from Mo doped ZIF-67: an effective catalyst for electrochemical H2O2 sensing. Microchem J 185:108296

    CAS  Google Scholar 

  • Saenz-Arana R, Hernandez C, Guinto T, Ahsan MA, Kim H, Lin Y, Alvarado-Tenorio B, Noveron J (2018) Adsorption of methylene blue and tetracycline onto biomass-based material prepared by sulfuric acid reflux. RSC Adv 8:32545–32557

    Google Scholar 

  • Saghir S, Xiao Z (2021) Hierarchical mesoporous ZIF-67@LDH for efficient adsorption of aqueous Methyl Orange and Alizarine Red S. Powder Technol 377:453–463

    CAS  Google Scholar 

  • Sahoo SK, Padhiari S, Biswal SK, Panda BB, Hota G (2020) Fe3O4 nanoparticles functionalized GO/g-C3N4 nanocomposite: An efficient magnetic nanoadsorbent for adsorptive removal of organic pollutants. Mater Chem Phys 244:122710

    CAS  Google Scholar 

  • Shao Y, Tian M, Zhen Z, Cui J, Xiao M, Qi B, Wang T, Hou X (2022) Adsorption of Ag/Au nanoparticles by ordered macro-microporous ZIF-67, and their synergistic catalysis application. J Clean Prod 346:131032

    CAS  Google Scholar 

  • Tang M, Li F, Yang M, Zhang Y (2020) Degradation of kanamycin from production wastewater with high-concentration organic matrices by hydrothermal treatment. J Environ Sci 97(14):11–18

    CAS  Google Scholar 

  • Tonda S, Kumar S, Bhardwaj M, Yadav P, Ogale S (2018) g-C3N4/NiAl-LDH 2D/2D hybrid heterojunction for high-performance photocatalytic reduction of CO2 into renewable fuels. ACS Appl Mater Interfaces 10(3):2667–2678

    CAS  Google Scholar 

  • Wang C-C, Yi X-H, Wang P (2019) Powerful combination of MOFs and C3N4 for enhanced photocatalytic performance. Appl Catal B 247:24–48

    CAS  Google Scholar 

  • Wang Q, Zhang Z, Shi S, Wu F, Zhang Z, Li G, Suo Y (2021) Highly active cobalt- and nitrogen-doped carbon derived from ZIF-67@melamine towards oxygen reduction reaction. J Electroanal Chem 894:115397

    CAS  Google Scholar 

  • Wang T, Xue L, Liu Y, Zhang L, Xing B (2022) N self-doped hierarchically porous carbon derived from biomass as an efficient adsorbent for the removal of tetracycline antibiotics. Sci Total Environ 822:153567

    CAS  Google Scholar 

  • Wee L, Janssens N, Sree S, Wiktor C, Gobechiya E, Fischer R, Kirschhock C, Martens J (2014) Local transformation of ZIF-8 powders and coatings into ZnO nanorods for photocatalytic application. Nanoscale 6:2056–2060

    CAS  Google Scholar 

  • Wu M-H, Li L, Xue Y-C, Xu G, Tang L, Liu N, Huang W-Y (2018) Fabrication of ternary GO/g-C3N4/MoS2 flower-like heterojunctions with enhanced photocatalytic activity for water remediation. Appl Catal B 228:103–112

    CAS  Google Scholar 

  • Wu M, Zhai M, Li X (2021) Adsorptive removal of oil drops from ASP flooding-produced water by polyether polysiloxane-grafted ZIF-8. Powder Technol 378:76–84

    CAS  Google Scholar 

  • Xu R, Yang Z-H, Zheng Y, Zhang H-B, Liu J-B, Xiong W-P, Zhang Y-R, Ahmad K (2017) Depth-resolved microbial community analyses in the anaerobic co-digester of dewatered sewage sludge with food waste. Biores Technol 244:824–835

    CAS  Google Scholar 

  • Yi L, Zuo L, Wei C, Fu H, Qu X, Zheng S, Xu Z, Guo Y, Li H, Zhu D (2020) Enhanced adsorption of bisphenol A, tylosin, and tetracycline from aqueous solution to nitrogen-doped multiwall carbon nanotubes via cation-π and π-π electron-donor-acceptor (EDA) interactions. Sci Total Environ 719:137389

    CAS  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

    CAS  Google Scholar 

  • Yu Y, Chen D, Xu W, Fang J, Sun J, Liu Z, Chen Y, Liang Y, Fang Z (2021) Synergistic adsorption-photocatalytic degradation of different antibiotics in seawater by a porous g-C3N4/calcined-LDH and its application in synthetic mariculture wastewater. J Hazard Mater 416:126183

    CAS  Google Scholar 

  • Zhu B, Xia P, Ho W, Yu J (2015) Isoelectric point and adsorption activity of porous g-C3N4. Appl Surf Sci 344:188–195

    CAS  Google Scholar 

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Funding

This work is financially supported by the Special Project for Performance Guidance of Scientific Institutions in Chongqing (No. 19237), National Defense Science and Technology Innovation Fund of the Chinese Academy of Sciences (No. NTCIP-XD/B07 (22607)), and the Postdoctoral Science Foundation of Shananxi Province (No. 282672, No. 285006).

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All authors contributed to the study conception and design. Specific contributions for each author are as follows. Mingyuan Zhang: writing—original draft. Yueyao Li: writing—reviewing. Xiaoying Zhou: reviewing and editing. Chentao Hou: supervision. Yuke Xie: investigation. Liping Wang: supervision, project administration, funding acquisition.

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Correspondence to Chentao Hou.

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Zhang, M., Li, Y., Zhou, X. et al. Preparation of ZIF-67/C3N4 composite material and adsorption of tetracycline hydrochloride. Environ Sci Pollut Res 30, 94112–94125 (2023). https://doi.org/10.1007/s11356-023-28919-6

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