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Co-doped Fe-MIL-100 as an adsorbent for tetracycline removal from aqueous solution

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Abstract

In the study, Fe-MIL-100 was modified by adding Co2+ in the synthesis process; Co/Fe-MIL-100 was successfully synthesized and used to adsorb tetracycline. The addition of Co2+ increased the thermal stability of Fe-MIL-100 without changing the crystal structure. It was found that Co/Fe-MIL-100 exhibited satisfactory performance in tetracycline removal, the tetracycline removal efficiency reached almost 100% in the initial concentration range of 10–40 mg/L, and it still reached 82.38% under the condition of 60 mg/L tetracycline. Besides, the factors of tetracycline concentration, pH and inorganic anion on removal efficiency were explored. The coexistence of inorganic anion decreased the adsorption capacity of tetracycline due to the competitive adsorption. CO32− had a more obvious inhibition effect on the adsorption efficiency of tetracycline than Cl−. The fitting correlation coefficient of Langmuir model was higher and the kinetics better fitted by pseudo-second-order, respectively. As a result of its high removal efficiency and excellent recycling performance, it has great potential in application fields such as removing tetracycline from wastewater.

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The datasets are available from the corresponding author on formal and logic request.

References

  • Alothman ZA, AlMasoud N, Mbianda XY, Ali I (2021) Synthesis and characterization of γ-cyclodextrin-graphene oxide nanocomposite: sorption, kinetics, thermodynamics and simulation studies of tetracycline and chlortetracycline antibiotics removal in water. J Mol Liq 345:116993

  • Chávez AM, Rey A, López J, Álvarez PM, Beltrán FJ (2021) Critical aspects of the stability and catalytic activity of MIL-100(Fe) in different advanced oxidation processes. Sep Purif Technol 255:117660

    Article  CAS  Google Scholar 

  • Chen L, Wang X, Rao Z, Tang Z, Wang Y, Shi G, Lu G, Xie X, Chen D, Sun J (2021) In-situ synthesis of Z-scheme MIL-100(Fe)/α-Fe2O3 heterojunction for enhanced adsorption and visible-light photocatalytic oxidation of O-xylene. Chem Eng J 416:129112

    Article  CAS  Google Scholar 

  • Chen S, Zang Z, Zhang S, Ouyang G, Han R (2021) Preparation of MIL-100(Fe) and multi-walled carbon nanotubes nanocomposite with high adsorption capacity towards oxytetracycline from solution. J Environ Chem Eng 9(2):104780

    Article  CAS  Google Scholar 

  • Chen W, Zhao B, Guo Y, Guo Y, Zheng Z, Pak T, Li G (2021) Effect of hydrothermal pretreatment on pyrolyzed sludge biochars for tetracycline adsorption. J Environ Chem Eng 9(6):106557

    Article  CAS  Google Scholar 

  • Dotto GL, McKay G (2020) Current scenario and challenges in adsorption for water treatment. J Environ Chem Eng 8(4):103988

    Article  CAS  Google Scholar 

  • Fan X, Hu H, Qin J, Cao X, Zhao R, Wang D (2021) Mechanism study on NO removal over the CQDs@MIL-100 (Fe) composite photocatalyst. Environ Technol Innov 24:101809

    Article  CAS  Google Scholar 

  • Flores JG, Díaz-García M, Ibarra IA, Aguilar-Pliego J, Sánchez-Sánchez M (2021) Sustainable M-MOF-74 (M = Cu Co, Zn) prepared in methanol as heterogeneous catalysts in the synthesis of benzaldehyde from styrene oxidation. J Solid State Chem 298:122151

    Article  CAS  Google Scholar 

  • Forghani M, Azizi A, Livani MJ, Kafshgari LA (2020) Adsorption of lead(II) and chromium(VI) from aqueous environment onto metal-organic framework MIL-100(Fe): synthesis, kinetics, equilibrium and thermodynamics. J Solid State Chem 291:121636

    Article  CAS  Google Scholar 

  • Gnanasekaran G, Sudhakaran MSP, Kulmatova D, Han J, Arthanareeswaran G, Jwa E, Mok YS (2021) Efficient removal of anionic, cationic textile dyes and salt mixture using a novel CS/MIL-100 (Fe) based nanofiltration membrane. Chemosphere 284:131244

    Article  CAS  Google Scholar 

  • Guo J, Jia H, Zhang A, Pei Z, Luo M, Xue J, Shen Q, Liu X, Xu B (2021) MIL-100 (Fe) with mix-valence coordinatively unsaturated metal site as Fenton-like catalyst for efficiently removing tetracycline hydrochloride: boosting Fe(III)/Fe(II) cycle by photoreduction. Sep Purif Technol 262:118334

    Article  CAS  Google Scholar 

  • Hachemaoui M, Mokhtar A, Ismail I, Mohamedi MW, Iqbal J, Taha I, Bennabi F, Zaoui F, Bengueddach A, Hamacha R, Boukoussa B (2021) M (M: Cu Co, Cr or Fe) nanoparticles-loaded metal-organic framework MIL-101(Cr) material by sonication process: catalytic activity and antibacterial properties. Microporous Mesoporous Mater 323:111244

    Article  CAS  Google Scholar 

  • Hameedi IT (2021) Determination of tetracycline hydrochloride in pure and pharmaceutical samples via oxidative coupling reaction. Materials Today: Proceedings 42:2953–2958

    CAS  Google Scholar 

  • Hasan Z, Jhung SH (2015) Removal of hazardous organics from water using metal-organic frameworks (MOFs): plausible mechanisms for selective adsorptions. J Hazard Mater 283:329–339

    Article  CAS  Google Scholar 

  • He Y, Dong W, Li X, Wang D, Yang Q, Deng P, Huang J (2020) Modified MIL-100(Fe) for enhanced photocatalytic degradation of tetracycline under visible-light irradiation. J Colloid Interface Sci 574:364–376

    Article  CAS  Google Scholar 

  • Hoslett J, Ghazal H, Katsou E, Jouhara H (2021) The removal of tetracycline from water using biochar produced from agricultural discarded material. Sci Total Environ 751:141755

    Article  CAS  Google Scholar 

  • Huang X, Yu S, Lin W, Yao X, Zhang M, He Q, Fu F, Zhu H, Chen J (2021) A metal-organic framework MIL-53(Fe) containing sliver ions with antibacterial property. J Solid State Chem 302:122442

    Article  CAS  Google Scholar 

  • Jang HY, Kang JK, Park JA, Lee SC, Kim SB (2020) Metal-organic framework MIL-100(Fe) for dye removal in aqueous solutions: prediction by artificial neural network and response surface methodology modeling. Environ Pollut 267:115583

    Article  CAS  Google Scholar 

  • Jang H-Y, Kang J-K, Lee S-C, Park J-A, Kim S-B (2021) Analysis of diclofenac removal by metal-organic framework MIL-100(Fe) using multi-parameter experiments and artificial neural network modeling. J Taiwan Inst Chem Eng 121:257–267

    Article  CAS  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

    Article  CAS  Google Scholar 

  • Li W, Zhang T, Lv L, Chen Y, Tang W, Tang S (2021) Room-temperature synthesis of MIL-100(Fe) and its adsorption performance for fluoride removal from water. Colloids Surf A: Physicochem Eng Asp 624:126791

    Article  CAS  Google Scholar 

  • Li Y, Lin X, Zhang C, Zhuang Q, Dong W (2021) Polydopamine magnetic microspheres grafted with sulfonic acid groups for efficient adsorption of tetracycline. Colloids Surf A: Physicochem Eng Asp 628:127263

    Article  CAS  Google Scholar 

  • Li X, Xu J, Shi J, Luo X (2022) Rapid and efficient adsorption of tetracycline from aqueous solution in a wide pH range by using iron and aminoacetic acid sequentially modified hierarchical porous biochar. Bioresour Technol 346:126672

    Article  CAS  Google Scholar 

  • Lian S, Shi X, Lu M, Zhang M, Dong X, Li X, Feng Q, Guo R (2021) Accelerated adsorption of tetracyclines and microbes with FeOn(OH)m modified oyster shell: its application on biotransformation of oxytetracycline in anaerobic enrichment culture. Chem Eng J 425:130499

    Article  CAS  Google Scholar 

  • Liao Q, Rong H, Zhao M, Luo H, Chu Z, Wang R (2022) Strong adsorption properties and mechanism of action with regard to tetracycline adsorption of double-network polyvinyl alcohol-copper alginate gel beads. J Hazard Mater 422:126863

    Article  CAS  Google Scholar 

  • Mahmoudi F, Amini MM, Sillanpää M (2020) Hydrothermal synthesis of novel MIL-100(Fe)@SBA-15 composite material with high adsorption efficiency towards dye pollutants for wastewater remediation. J Taiwan Inst Chem Eng 116:303–313

    Article  CAS  Google Scholar 

  • Martinez-Carballo E, Gonzalez-Barreiro C, Scharf S, Gans O (2007) Environmental monitoring study of selected veterinary antibiotics in animal manure and soils in Austria. Environ Pollut 148:570–579

    Article  CAS  Google Scholar 

  • Mehrtens A, Licha T, Broers HP, Burke V (2020) Tracing veterinary antibiotics in the subsurface - a long-term field experiment with spiked manure. Environ Pollut 265:114930

    Article  CAS  Google Scholar 

  • Niu L, Zhang G, Xian G, Ren Z, Wei T, Li Q, Zhang Y, Zou Z (2021) Tetracycline degradation by persulfate activated with magnetic γ-Fe2O3/CeO2 catalyst: performance, activation mechanism and degradation pathway. Sep Purif Technol 259:118156

    Article  CAS  Google Scholar 

  • Omer AM, Abd El-Monaem EM, El-Subruiti GM, Abd El-Latif MM, Eltaweil AS (2021) Fabrication of easy separable and reusable MIL-125(Ti)/MIL-53(Fe) binary MOF/CNT/Alginate composite microbeads for tetracycline removal from water bodies. Sci Rep 11:23818

    Article  CAS  Google Scholar 

  • Ouaissa YA, Chabani M, Amrane A, Bensmaili A (2014) Removal of tetracycline by electrocoagulation: kinetic and isotherm modeling through adsorption. J Environ Chem Eng 2:177–184

    Article  CAS  Google Scholar 

  • Paula Fagundes A, Viana Felipe, da Silva A, Bueno de Morais B, Lusitâneo Pier Macuvele D, Nones J, GracherRiella H, Padoin N, Soares C (2021) A novel application of bentonite modified with copper ions in the tetracycline adsorption: an experimental design study. Mater Lett 291:129552

    Article  CAS  Google Scholar 

  • Qiao H, Wang X, Liao P, Zhang C, Liu C (2021) Enhanced sequestration of tetracycline by Mn(II) encapsulated mesoporous silica nanoparticles: synergistic sorption and mechanism. Chemosphere 284:131334

    Article  CAS  Google Scholar 

  • Seo Y-K, Yoon JW, Lee JS, Lee UH, Hwang YK, Jun C-H, Horcajada P, Serre C, Chang J-S (2012) Large scale fluorine-free synthesis of hierarchically porous iron(III) trimesate MIL-100(Fe) with a zeolite MTN topology. Microporous Mesoporous Mater 157:137–145

    Article  CAS  Google Scholar 

  • Song J, Huang M, Lin X, Li SFY, Jiang N, Liu Y, Guo H, Li Y (2022) Novel Fe-based metal–organic framework (MOF) modified carbon nanofiber as a highly selective and sensitive electrochemical sensor for tetracycline detection. Chem Eng J 427:130913

    Article  CAS  Google Scholar 

  • Tang Y, Huang X, Wang X, Wang C, Tao H, Wu Y (2021) G-quadruplex DNAzyme as peroxidase mimetic in a colorimetric biosensor for ultrasensitive and selective detection of trace tetracyclines in foods. Food Chem 366:130560

    Article  CAS  Google Scholar 

  • Tian N, Jia Q, Su H, Zhi Y, Ma A, Wu J, Shan S (2016) The synthesis of mesostructured NH2-MIL-101(Cr) and kinetic and thermodynamic study in tetracycline aqueous solutions. J Porous Mater 23:1269–1278

    Article  CAS  Google Scholar 

  • Van Boeckel TP, Brower C, Gilbert M, Grenfell BT, Levin SA, Robinson TP, Teillant A, Laxminarayan R (2015) Global trends in antimicrobial use in food animals. Proc Natl Acad Sci 112:5649–5654

    Article  CAS  Google Scholar 

  • Wang H, Yuan X, Wu Y, Zeng G, Dong H, Chen X, Leng L, Wu Z, Peng L (2016) In situ synthesis of In2S3@MIL-125(Ti) core–shell microparticle for the removal of tetracycline from wastewater by integrated adsorption and visible-light-driven photocatalysis. Appl Catal B 186:19–29

    Article  CAS  Google Scholar 

  • Wang D, Jia F, Wang H, Chen F, Fang Y, Dong W, Zeng G, Li X, Yang Q, Yuan X (2018) Simultaneously efficient adsorption and photocatalytic degradation of tetracycline by Fe-based MOFs. J Colloid Interface Sci 519:273–284

    Article  CAS  Google Scholar 

  • Wang Z, Chen Q, Zhang J, Dong J, Yan H, Chen C, Feng R (2019) Characterization and source identification of tetracycline antibiotics in the drinking water sources of the lower Yangtze River. J Environ Manage 244:13–22

    Article  CAS  Google Scholar 

  • Wu J, Gao Y, Wei S, Chen P, Gu D, Fu B, Chen M (2021) Plasma modification of Fe-MOF for efficient organic pollutants removal. J Solid State Chem 302:122350

    Article  CAS  Google Scholar 

  • Wu L, Wang CC, Chu HY, Yi XH, Wang P, Zhao C, Fu H (2021) Bisphenol A cleanup over MIL-100(Fe)/CoS composites: pivotal role of Fe-S bond in regenerating Fe(2+) ions for boosted degradation performance. Chemosphere 280:130659

    Article  CAS  Google Scholar 

  • Xia L, Luan X, Qu F, Lu L (2020) Co-MOF/titanium nanosheet array: an excellent electrocatalyst for non-enzymatic detection of H2O2 released from living cells. J Electroanalyt Chem 878:114553

    Article  CAS  Google Scholar 

  • Xiong W, Zeng G, Yang Z, Zhou Y, Zhang C, Cheng M, Liu Y, Hu L, Wan J, Zhou C, Xu R, Li X (2018) Adsorption of tetracycline antibiotics from aqueous solutions on nanocomposite multi-walled carbon nanotube functionalized MIL-53(Fe) as new adsorbent. Sci Total Environ 627:235–244

    Article  CAS  Google Scholar 

  • Xiong W, Zeng Z, Li X, Zeng G, Xiao R, Yang Z, Xu H, Chen H, Cao J, Zhou C, Qin L (2019) Ni-doped MIL-53(Fe) nanoparticles for optimized doxycycline removal by using response surface methodology from aqueous solution. Chemosphere 232:186–194

    Article  CAS  Google Scholar 

  • Yu C, Gou L, Zhou X, Bao N, Gu H (2011) Chitosan–Fe3O4 nanocomposite based electrochemical sensors for the determination of bisphenol A. Electrochim Acta 56:9056–9063

    Article  CAS  Google Scholar 

  • Yue Y, Liu YJ, Wang J, Vukanti R, Ge Y (2021) Enrichment of potential degrading bacteria accelerates removal of tetracyclines and their epimers from cow manure biochar amended soil. Chemosphere 278:130358

    Article  CAS  Google Scholar 

  • Zhai W, He J, Han P, Zeng M, Gao X, He Q (2022) Adsorption mechanism for tetracycline onto magnetic Fe3O4 nanoparticles: adsorption isotherm and dynamic behavior, location of adsorption sites and interaction bonds. Vacuum 195:110634

    Article  CAS  Google Scholar 

  • Zhang F, Shi J, Jin Y, Fu Y, Zhong Y, Zhu W (2015) Facile synthesis of MIL-100(Fe) under HF-free conditions and its application in the acetalization of aldehydes with diols. Chem Eng J 259:183–190

    Article  CAS  Google Scholar 

  • Zhang G, Chen S, Yang Y, Liu Y, Lei L, Liu X, Xiao R, Du L, Huang D, Cheng M (2021) Boron nitride quantum dots decorated MIL-100(Fe) for boosting the photo-generated charge separation in photocatalytic refractory antibiotics removal. Environ Res 202:111661

    Article  CAS  Google Scholar 

  • Zhao Y, Geng J, Wang X, Gu X, Gao S (2011) Adsorption of tetracycline onto goethite in the presence of metal cations and humic substances. J Colloid Interface Sci 361:247–251

    Article  CAS  Google Scholar 

  • Zhao X, Wang J, Zhu L, Ge W, Wang J (2017) Environmental analysis of typical antibiotic-resistant bacteria and ARGs in farmland soil chronically fertilized with chicken manure. Sci Total Environ 593–594:10–17

    Article  CAS  Google Scholar 

  • Zhou D, Chen X, Liang B, Fan X, Wei X, Liang J, Wang L (2019) Embedding MIL-100(Fe) with magnetically recyclable Fe3O4 nanoparticles for highly efficient esterification of diterpene resin acids and the associated kinetics. Microporous Mesoporous Mater 289:109615

    Article  CAS  Google Scholar 

  • Zhu D, Cai L, Sun Z, Zhang A, Heroux P, Kim H, Yu W, Liu Y (2021) Efficient degradation of tetracycline by RGO@black titanium dioxide nanofluid via enhanced catalysis and photothermal conversion. Sci Total Environ 787:147536

    Article  CAS  Google Scholar 

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Funding

This work was supported by the Research Project of Shanghai Waterway Engineering Design and Consulting Company (2021-431 J,2020-231 J), Research Project of CCCC Shanghai Dredging Company (2020-199 J).

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Authors and Affiliations

  1. Shanghai Waterway Engineering Design and Consulting Co., Ltd., Shanghai, 200120, China

    Feiyue Jia, Donghua Zhao, Mengzhao Shu, Feifei Sun, Chen Chen, Yu Deng & Xiaoming Zhu

  2. College of Environmental Science and Engineering, Hunan University, Changsha, 410082, People’s Republic of China

    Dongbo Wang

  3. Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, Hunan University, Changsha, 410082, People’s Republic of China

    Dongbo Wang

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  1. Feiyue Jia
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  2. Donghua Zhao
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  3. Mengzhao Shu
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  4. Feifei Sun
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  5. Dongbo Wang
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  6. Chen Chen
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  7. Yu Deng
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  8. Xiaoming Zhu
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Contributions

FJ contributed to conceptualization, investigation, and writing of the original draft. YD and MS contributed in language modification. FS and CC made literature research and conducted validation. DZ and XZ contributed to methodology and DW contributed to review.

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Correspondence to Dongbo Wang.

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Jia, F., Zhao, D., Shu, M. et al. Co-doped Fe-MIL-100 as an adsorbent for tetracycline removal from aqueous solution. Environ Sci Pollut Res 29, 55026–55038 (2022). https://doi.org/10.1007/s11356-022-19684-z

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