Skip to main content
Springer Nature Link
Log in

Preparation, characterization, and catalytic activity of a novel MgO/expanded graphite for ozonation of Cu-EDTA

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Magnesium oxide/expanded graphite (MgO/EG) catalyst was synthesized and applied for enhancing the degradation of Cu-ethylenediaminetetraacetic acid (Cu-EDTA) in an aqueous solution. The MgO/EG catalyst was characterized by XRD, SEM, EDS, and FTIR. For assessing the catalytic activity of MgO/EG, essential influencing factors were investigated including catalyst dosage, O3 dosage, initial pH, initial Cu-EDTA concentration, and coexisting ions. The results show that the catalytic material showed high catalytic oxidation capacity for the Cu-EDTA removal in the MgO/EG/O3 system. 100% of Cu(II) and 73.2% of TOC removal efficiency could be achieved in the MgO/EG/O3 system at the reaction times of 90 min. This efficiency was higher than that seen for other systems, including O3 alone (Cu(II) 81.4%/TOC 60.6%), EG/O3 (84.2%/64.1), MgO/EG (< 4%/< 4%), and EG (< 4%/< 4%). A small decrease in the Cu(II) and TOC removal rate was observed after three runs in the stability and reusability experiments of the catalyst. Assays with radical scavenging experiments confirmed that MgO/EG-mediated oxidation was dependent on a hydroxyl radical pathway. The UV–vis spectra confirmed that the absorption peak of Cu-EDTA was gradually decreased and finally disappeared.

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

Access this article

Log in via an institution

Subscribe and save

Springer+ Basic
$34.99 /Month
  • Get 10 units per month
  • Download Article/Chapter or eBook
  • 1 Unit = 1 Article or 1 Chapter
  • Cancel anytime
Subscribe now

Buy Now

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

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8

Similar content being viewed by others

Explore related subjects

Discover the latest articles and news from researchers in related subjects, suggested using machine learning.

Availability of data and materials

All data generated or analyzed during this study are included in this published article.

References

  • Alinejad A, Akbari H, Ghaderpoori M, Jeihooni AK, Adibzadeh A (2019) Catalytic ozonation process using a MgO nano-catalyst to degrade methotrexate from aqueous solutions and cytotoxicity studies in human lung epithelial cells (A549) after treatment. RSC Adv 9:8204–8214

    Article  CAS  Google Scholar 

  • Bader H, Hoigné J (1981) Determination of ozone in water by the indigo method. Water Res 15(4):449–456

    Article  CAS  Google Scholar 

  • Chen H, Wang J (2019) Catalytic ozonation of sulfamethoxazole over Fe3O4/Co3O4 composites. Chemosphere 234:14–24

    Article  CAS  Google Scholar 

  • Chen J, Tian S, Lu J, Xiong Y (2015) Catalytic performance of MgO with different exposed crystal facets towards the ozonation of 4-chlorophenol. Appl Catal A Gen 506:118–125

    Article  CAS  Google Scholar 

  • Chung DDL (2016) A review of exfoliated graphite. J Mater Sci 51:554–568

    Article  CAS  Google Scholar 

  • Durante C, Cuscov M, Isse AA, Sandonà G, Gennaro A (2011) Advanced oxidation processes coupled with electrocoagulation for the exhaustive abatement of Cr-EDTA. Water Res 45(5):2122–2130

    Article  CAS  Google Scholar 

  • Guan W, Zhang B, Tian S, Zhao X (2018) The synergism between electro-Fenton and electrocoagulation process to remove Cu-EDTA. Appl Catal B Environ 227:252–257

    Article  CAS  Google Scholar 

  • Guan Z, Guo Y, Li S, Feng S, Deng Y, Ou X, Ren J, Sun S, Liang J (2020) Decomplexation of heterogeneous catalytic ozonation assisted with heavy metal chelation for advanced treatment of coordination complexes of Ni. Sci Total Environ 732:139223

    Article  CAS  Google Scholar 

  • Guo H, Jiang N, Wang H, Shang K, Lu N, Li J, Wu Y (2019) Enhanced catalytic performance of graphene-TiO2 nanocomposites for synergetic degradation of fluoroquinolone antibiotic in pulsed discharge plasma system. Appl Catal B Environ 248:552–566

    Article  CAS  Google Scholar 

  • He J, Song L, Yang H, Ren X, Xing L (2017) Preparation of sulfur-Free exfoliated graphite by a two-step intercalation process and its application for adsorption of oils. J Chem 2017:1–8

    Google Scholar 

  • He J, Chen S, Yang S, Song W, Yu C, Song L (2020a) Fabrication of MoS2 loaded on expanded graphite matrix for high-efficiency pH-universal hydrogen evolution reaction. J Alloys Compd 828:154370

    Article  CAS  Google Scholar 

  • He J, Song W, Gao Z, Huang X (2020b) Calcium carbonate/expanded graphite as an efficient catalyst for catalytic ozonation of ethylenediaminetetraacetic acid. Environ Eng Sci 37(6):450–456

    Article  CAS  Google Scholar 

  • Huang X, Xu Y, Shan C, Li X, Zhang W, Pan B (2016) Coupled Cu(II)-EDTA degradation and Cu(II) removal from acidic wastewater by ozonation: performance, products and pathways. Chem Eng J 299:23–29

    Article  CAS  Google Scholar 

  • Jiraroj D, Unob F, Hagège A (2006) Degradation of Pb-EDTA complex by a H2O2/UV process. Water Res 40(1):107–112

    Article  CAS  Google Scholar 

  • Ju F, Hu Y (2011) Removal of EDTA-chelated copper from aqueous solution by interior microelectrolysis. Sep Purif Technol 78(1):33–41

    Article  CAS  Google Scholar 

  • Kalantary R, R, Moradi M, Pirsaheb M, Esrafili A, Jafari AJ, Gholami M, Vasseghian Y, Antolini E, Dragoi EN (2019) Enhanced photocatalytic inactivation of E. coli by natural pyrite in presence of citrate and EDTA as effective chelating agents: Experimental evaluation and kinetic and ANN models. J Environ Chem Eng 7(1):102906

  • Kamarehie B, Jafari A, Ghaderpoori M, Karami MA, Mousavi K, Ghaderpoury A (2019) Catalytic ozonation process using PAC/γ-Fe2O3 to Alizarin Red S degradation from aqueous solutions: a batch study. Chem Eng Commun 206:898–908

    Article  CAS  Google Scholar 

  • Lan S, Xiong Y, Tian S, Feng J, Xie T (2016) Enhance self-catalytic degradation of Cu-EDTA in the presence of H2O2/UV: evidence and importance of Cu-peroxide as a photo-active intermediate. Appl Catal B Environ 183:371–376

    Article  CAS  Google Scholar 

  • Li W, Qiang Z, Zhang T, Cao F (2012) Kinetics and mechanism of pyruvic acid degradation by ozone in the presence of PdO/CeO2. Appl Catal B Environ 113-114:290–295

    Article  CAS  Google Scholar 

  • Liu Z, Tu J, Wang Q, Cui Y, Zhang L, Wu X, Zhang B, Ma J (2018) Catalytic ozonation of diethyl phthalate in aqueous solution using graphite supported zinc oxide. Sep Purif Technol 200:51–58

    Article  CAS  Google Scholar 

  • Mashayekh-Salehi A, Moussavi G, Yaghmaeian K (2017) Preparation, characterization and catalytic activity of a novel mesoporous nanocrystalline MgO nanoparticle for ozonation of acetaminophen as an emerging water contaminant. Chem Eng J 310:157–169

    Article  CAS  Google Scholar 

  • Meng X, Liu Z, Deng C, Zhu M, Wang D, Li K, Deng Y, Jiang M (2016) Microporous nano-MgO/diatomite ceramic membrane with highpositive surface charge for tetracycline removal. J Hazard Mater 320:495–503

    Article  CAS  Google Scholar 

  • Miklos DB, Remy C, Jekel M, Linden KG, Drewes JE, Hübner U (2018) Evaluation of advanced oxidation processes for water and wastewater treatment-A critical review. Water Res 139(1):118–131

    Article  CAS  Google Scholar 

  • Moradi M, Elahinia A, Vasseghian Y, Dragoi EN, Omidi F, Khaneghah AM (2020a) A review on pollutants removal by Sono-photo -Fenton processes. J Environ Chem Eng 8(5):104330

    Article  CAS  Google Scholar 

  • Moradi M, Vasseghian Y, Khataee A, Kobya M, Arabzade H, Dragoi EN (2020b) Service life and stability of electrodes applied in electrochemical advanced oxidation processes: a comprehensive review. J Ind Eng Chem 87:18–39

    Article  CAS  Google Scholar 

  • Moradi M, Vasseghian Y, Khataee A, Harati M, Arfaeinia H (2021) Ultrasound-assisted synthesis of FeTiO3/GO nanocomposite for photocatalytic degradation of phenol under visible light irradiation. Sep Purif Technol 261:118274

    Article  CAS  Google Scholar 

  • Moussavi G, Mahmoudi M (2019) Degradation and biodegradability improvement of the reactive red 198 azo dye using catalytic ozonation with MgO nanocrystals. Chem Eng J 152:1–7

    Article  Google Scholar 

  • Moussavi G, Aghapour AA, Yaghmaeian K (2014) The degradation and mineralization of catechol using ozonation catalyzed with MgO/GAC composite in a fluidized bed reactor. Chem Eng J 249:302–310

    Article  CAS  Google Scholar 

  • Nasseh N, Arghavan FS, Rodriguez-Couto S, Panahi AH, Esmati M, A-Musawi TJ (2020) Preparation of activated carbon@ZnO composite and its application as a novel catalyst in catalytic ozonation process for metronidazole degradation. Adv Powder Technol 31(2):875–885

    Article  CAS  Google Scholar 

  • Nawrocki J, Kasprzyk-Hordern B (2010) The efficiency and mechanisms of catalytic ozonation. Appl Catal B Environ 99(1-2):27–42

    Article  CAS  Google Scholar 

  • Oturan MA, Aaron JJ (2014) Advanced oxidation processes in water/wastewater treatment: principles and applications. a review. Crit Rev Environ Sci Technol 44:2577–2641

    Article  CAS  Google Scholar 

  • Qiu W, Zheng M, Sun J, Tian Y, Fang M, Zheng Y, Zhang T, Zheng C (2019) Photolysis of enrofloxacin, pefloxacin and sulfaquinoxaline in aqueous solution by UV/H2O2, UV/Fe(II), and UV/H2O2/Fe(II) and the toxicity of the final reaction solutions on zebrafish embryos. Sci Total Environ 651:1457–1468

    Article  CAS  Google Scholar 

  • Restivo J, Órfão JJM, Pereira MFR, Garcia-Bordejé E, Roche P, Bourdin D, Houssais B, Coste M, Derrouiche S (2013) Catalytic ozonation of organic micropollutants using carbon nanofibers supported on monoliths. Chem Eng J 230:115–123

    Article  CAS  Google Scholar 

  • Wang T, Cao Y, Qu G, Sun Q, Xia T, Guo X, Jia H, Zhu L (2018) Novel Cu(II)-EDTA decomplexation by discharge plasma oxidation and coupled Cu removal by alkaline precipitation: underneath mechanisms. Environ Sci Technol 52(14):7884–7891

    Article  CAS  Google Scholar 

  • Wei K, Cao X, Gu W, Liang P, Oturan X, Zhang X (2019) Ni-induced C-Al2O3-framework (NiCAF) supported core-multishell catalysts for efficient catalytic ozonation: a structure-to-performance study. Environ Sci Technol 53(12):6917–6926

    Article  CAS  Google Scholar 

  • Xie W, Zhou F, Bi X, Chen D, Huang Z, Li Y, Sun S, Liu J (2019) Decomposition of Nickel(II)-Ethylenediaminetetraacetic acid by Fenton-like reaction over oxygen vacancies-based Cu-Doped Fe3O4@γ-Al2O3 catalyst: a synergy of oxidation and adsorption. Chemosphere 221:563–572

    Article  CAS  Google Scholar 

  • Xu M, Li J, Yan Y, Zhao X, Yan J, Zhang Y, Lai B, Chen X, Song L (2019) Catalytic degradation of sulfamethoxazole through peroxymonosulfate activated with expanded graphite loaded CoFe2O4 particles. Chem Eng J 369:403–413

    Article  CAS  Google Scholar 

  • Yang JK, Davis AP (2000) Photocatalytic oxidation of Cu(II)-EDTA with illuminated TiO2: mechanisms. Environ Sci Technol 34(17):3796–3801

    Article  CAS  Google Scholar 

  • Yang Y, Cao H, Peng P, Bo H (2014) Degradation and transformation of atrazine under catalyzed ozonation process with TiO2 as catalyst. J Hazard Mater 279:444–451

    Article  CAS  Google Scholar 

  • Yang Y, Zhang P, Jia J (2019) Vanadium-doped MnO2 for efficient room-temperature catalytic decomposition of ozone in air. Appl Surf Sci 484:45–53

    Article  CAS  Google Scholar 

  • Ye X, Zhang J, Zhang Y, Lv Y, Dou R, Wen S, Li L, Chen Y, Hu Y (2016) Treatment of Ni-EDTA containing wastewater by electrocoagulation using iron scraps packed-bed anode. Chemosphere 164:304–313

    Article  CAS  Google Scholar 

  • Yu X, Zhang Y, Cheng X (2014) Preparation and photoelectrochemical performance of expanded graphite/TiO2 composite. Electrochim Acta 137:668–675

    Article  CAS  Google Scholar 

  • Zhang G, Zhong J, Xu M, Yang Y, Li Y, Fang Z, Tang S, Yuan D, Wen B, Gu J (2019a) Ternary BiVO4/NiS/Au nanocomposites with efficient charge separations for enhanced visible light photocatalytic performance. Chem Eng J 375:122093

    Article  CAS  Google Scholar 

  • Zhang L, Wu B, Zhang G, Gan Y, Zhang S (2019b) Enhanced decomplexation of Cu(II)-EDTA: The role of acetylacetone in Cu-mediated photo-Fenton reactions. Chem Eng J 358:1218–1226

    Article  CAS  Google Scholar 

  • Zhou J, Yang S, Yu J (2011) Facile fabrication of mesoporous MgO microspheres and their enhanced adsorption performance for phosphate from aqueous solutions. Colloids Surf A Physicochem Eng Asp 379(1-3):102–108

    Article  CAS  Google Scholar 

Download references

Funding

This work was supported by the Natural Science Foundation of Hebei Province (No. B2020203013).

Author information

Authors and Affiliations

  1. School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao, 066004, China

    Jun He, Wenchao Song, Xiaohan Huang & Zuoyu Gao

  2. Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, Qinhuangdao, 066004, China

    Jun He, Wenchao Song, Xiaohan Huang & Zuoyu Gao

  3. Hebei Key Laboratory of Applied Chemistry, Qinhuangdao, 066004, China

    Jun He, Wenchao Song, Xiaohan Huang & Zuoyu Gao

Authors
  1. Jun He
    View author publications

    Search author on:PubMed Google Scholar

  2. Wenchao Song
    View author publications

    Search author on:PubMed Google Scholar

  3. Xiaohan Huang
    View author publications

    Search author on:PubMed Google Scholar

  4. Zuoyu Gao
    View author publications

    Search author on:PubMed Google Scholar

Contributions

All authors contributed to the study conception and design. Supervision, writing-review and editing: Jun He; methodology, formal analysis, data curation, writing-original draft: Wenchao Song; visualization, data curation: Xiaohan Huang; investigation, formal analysis: Zuoyu Gao. All authors read and approved the final manuscript.

Corresponding author

Correspondence to Jun He.

Ethics declarations

Ethics approval and consent to participate

Not applicable.

Consent for publication

Not applicable.

Conflict of interest

The authors declare no conflict of interest.

Additional information

Responsible Editor: Ricardo Torres-Palma

Publisher’s note

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

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

He, J., Song, W., Huang, X. et al. Preparation, characterization, and catalytic activity of a novel MgO/expanded graphite for ozonation of Cu-EDTA. Environ Sci Pollut Res 28, 39513–39523 (2021). https://doi.org/10.1007/s11356-021-13551-z

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-021-13551-z

Keywords