Skip to main content
SpringerLink
Log in

Enhanced removal of toxic hexavalent chromium from aqueous solution by magnetic Zr-MOF@polypyrrole: performance and mechanism

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

Abstract

Magnetic Zr–based metal organic framework (UiO-66) @Polypyrrole (magnetic UiO-66@Ppy) was prepared to eliminate Cr(VI) from water. SEM and TEM results clearly revealed that the magnetic UiO-66@Ppy was a core-double-shell structure with the core of Fe3O4, inner shell UiO-66, and outer shell Ppy. The introduction of zirconium MOFs UiO-66 effectively prevented the agglomeration of polypyrrole and provided more available adsorption sites, the surface area increased from 9.57 m2/g (Ppy) to 10.57 m2/g (Fe3O4@Ppy) and 52.49 m2/g (magnetic UiO-66@Ppy). The magnetic UiO-66@Ppy possessed a high adsorption capacity of 259.1 mg/g in removing Cr(VI) from water. Adsorption kinetics followed the pseudo-second-order model. The removal of Cr(VI) involved the following mechanisms: (1) electrostatic attraction and ions exchange, the HCrO4− was adsorbed on the surface of magnetic UiO-66@Ppy by the protonated N(PpyN+) and Cl−; (2) reduction, Cr(VI) was reduced to Cr(III) by the reductive functional group(-NH-); (3) chelation, Cr(III) was immobilized on adsorbent by amine groups.

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

Access this article

Log in via an institution

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
Fig. 9
Fig. 10
Fig. 11
Fig. 12
Fig. 13

Similar content being viewed by others

Data availability

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

References

  • Bajpai SK, Rohit VK, Namdeo M (2009) Removal of phosphate anions from aqueous solutions using polypyrrole-coated sawdust as a novel sorbent. J Appl Polym Sci 111:3081–3088

    Article  CAS  Google Scholar 

  • Bhaumik M, Maity A, Srinivasu VV, Onyango MS (2011) Enhanced removal of Cr(VI) from aqueous solution using polypyrrole/Fe3O4 magnetic nanocomposite. J Hazard Mater 190:381–390

    Article  CAS  Google Scholar 

  • Cai WQ, Wei JH, Li ZL, Liu Y, Zhou JB, Han BW (2019) Preparation of amino-functionalized magnetic biochar with excellent adsorption performance for Cr(VI) by a mild one-step hydrothermal method from peanut hull. Colloid Surface A 563:102–111

    Article  CAS  Google Scholar 

  • Chaudhuri RG, Paria S (2012) Core/shell nanoparticles: classes, properties, synthesis mechanisms, characterization, and applications. Chem Rev 112:2373–2433

    Article  Google Scholar 

  • Chavez-Guajardo AE, Medina-Llamas JC, Maqueira L, Andrade CAS, Alves KGB, de Melo CP (2015) Efficient removal of Cr (VI) and Cu (II) ions from aqueous media by use of polypyrrole/maghemite and polyaniline/maghemite magnetic nanocomposites. Chem Eng J 281:826–836

    Article  CAS  Google Scholar 

  • Chen CQ, Chen DZ, Xie SS, Quan HY, Luo XB, Guo L (2017) Adsorption behaviors of organic micropollutants on zirconium metal-organic framework UiO-66: analysis of surface interactions. ACS Appl Mater Interfaces 9:41043–41054

    Article  CAS  Google Scholar 

  • Dehghani MH et al (2015) Removal of noxious Cr (VI) ions using single-walled carbon nanotubes and multi-walled carbon nanotubes. Chem Eng J 279:344–352

    Article  CAS  Google Scholar 

  • Dotto GL, Cadaval TRS, Pinto LAA (2012) Preparation of bionanoparticles derived from Spirulina platensis and its application for Cr (VI) removal from aqueous solutions. J Ind Eng Chem 18:1925–1930

    Article  CAS  Google Scholar 

  • Dotto GL, Goncalves JO, Cadaval TRS, Pinto LAA (2013) Biosorption of phenol onto bionanoparticles from Spirulina sp LEB 18. J Colloid Interface Sci 407:450–456

    Article  CAS  Google Scholar 

  • Du LL, Gao P, Meng YD, Liu YL, Le SW, Yu CB (2020) Highly efficient removal of Cr(VI) from aqueous solutions by polypyrrole/monodisperse latex spheres. ACS Omega 5:6651–6660

    Article  CAS  Google Scholar 

  • Fang W, Jiang XY, Luo HJ, Geng JJ (2018) Synthesis of graphene/SiO2@polypyrrole nanocomposites and their application for Cr(VI) removal in aqueous solution. Chemosphere 197:594–602

    Article  CAS  Google Scholar 

  • Far HS, Hasanzadeh M, Nashtaei MS, Rabbani M, Haji A, Moghadam BH (2020) PPI-Dendrimer-functionalized magnetic metal-organic framework (Fe3O4@MOF@PPI) with high adsorption capacity for sustainable wastewater treatment. ACS Appl Mater Interfaces 12:25294–25303

    Article  CAS  Google Scholar 

  • Feng S, Wang RB, Feng SS, Zhang ZH, Liu SG (2018) Synthesis of UiO-66 based on benzoic acid and chloroform with highly efficient adsorption of Congo red dye. Desalin Water Treat 126:350–360

    Article  CAS  Google Scholar 

  • Hasan Z, Cho DW, Nam IH, Chon CM, Song H (2016) Preparation of calcined zirconia-carbon composite from metal organic frameworks and its application to adsorption of crystal violet and salicylic acid. Materials 9

  • Huang XP, Hou XJ, Song FH, Zhao JC, Zhang LZ (2016) Facet-dependent Cr(VI) adsorption of hematite nanocrystals. Environ Sci Technol 50:1964–1972

    Article  CAS  Google Scholar 

  • Huo JB, Xu L, Chen X, Zhang Y, Yang JCE, Yuan B, Fu ML (2019) Direct epitaxial synthesis of magnetic Fe3O4@UiO-66 composite for efficient removal of arsenate from water. Microporous Mesoporous Mater 276:68–75

    Article  CAS  Google Scholar 

  • Jadhav A, Gupta K, Ninawe P, Ballav N (2020) Imparting multifunctionality by utilizing biporosity in a zirconium-based metal-organic framework. Angew Chem Int Edit 59:2215–2219

    Article  CAS  Google Scholar 

  • Jagtap S, Yenkie MK, Labhsetwar N, Rayalus S (2012) Fluoride in drinking water and defluoridation of water. Chem Rev 112:2454–2466

    Article  CAS  Google Scholar 

  • Jamshidifard S, Koushkbaghi S, Hosseini S, Rezaei S, Karamipour A, Rad AJ, Irani M (2019) Incorporation of UiO-66-NH2 MOF into the PAN/chitosan nanofibers for adsorption and membrane filtration of Pb(II), Cd(II) and Cr(VI) ions from aqueous solutions. J Hazard Mater 368:10–20

    Article  CAS  Google Scholar 

  • Jang S et al (2019) Recent novel hybrid Pd-Fe3O4 nanoparticles as catalysts for various C-C coupling reactions. Processes 7

  • Kera NH, Bhaumik M, Pillay K, Ray SS, Maity A (2018) m-Phenylenediamine-modified polypyrrole as an efficient adsorbent for removal of highly toxic hexavalent chromium in water. Mater Today Commun 15:153–164

    Article  CAS  Google Scholar 

  • Lai YX et al (2019) UiO-66 derived N-doped carbon nanoparticles coated by PANI for simultaneous adsorption and reduction of hexavalent chromium from waste water. Chem Eng J 378

  • Li J et al (2019) The performance of UiO-66-NH2/graphene oxide (GO) composite membrane for removal of differently charged mixed dyes. Chemosphere 237

  • Li CY, Liu JM, Wang ZH, Lv SW, Zhao N, Wang S (2020a) Integration of Fe3O4@UiO-66-NH2@MON core-shell structured adsorbents for specific preconcentration and sensitive determination of aflatoxins against complex sample matrix. J Hazard Mater 384

  • Li LC, Xu YL, Zhong DJ, Zhong NB (2020b) CTAB-surface-functionalized magnetic MOF@MOF composite adsorbent for Cr(VI) efficient removal from aqueous solution. Colloid Surface A 586

  • Liang QW, Geng JJ, Luo HJ, Fang W, Yin YW (2017) Fast and selective removal of Cr(VI) from aqueous solutions by a novel magnetic Cr(VI) ion-imprinted polymer. J Mol Liq 248:767–774

    Article  CAS  Google Scholar 

  • Liang S et al (2019) One-pot solvothermal synthesis of magnetic biochar from waste biomass: Formation mechanism and efficient adsorption of Cr(VI) in an aqueous solution. Sci Total Environ 695:133886

    Article  CAS  Google Scholar 

  • Liu J et al (2009) Highly water-dispersible biocompatible magnetite particles with low cytotoxicity stabilized by citrate groups. Angew Chem Int Edit 48:5875–5879

    Article  CAS  Google Scholar 

  • Lutke SF, Igansi AV, Pegoraro L, Dotto GL, Pinto LAA, Cadaval TRS (2019) Preparation of activated carbon from black wattle bark waste and its application for phenol adsorption. J Environ Chem Eng 7

  • Lyu W et al (2019) Easy separated 3D hierarchical coral-like magnetic polyaniline adsorbent with enhanced performance in adsorption and reduction of Cr(VI) and immobilization of Cr(III). Chem Eng J 363:107–119

    Article  CAS  Google Scholar 

  • Mao H et al (2016) Hydrophilic polymer/polypyrrole/graphene oxide nanosheets with different performances in electrocatalytic applications to simultaneously determine dopamine and ascorbic acid. RSC Adv 6:111632–111639

    Article  CAS  Google Scholar 

  • Maurin G, Serre C, Cooper A, Fereyd G (2017) The new age of MOFs and of their porous-related solids. Chem Soc Rev 46:3104–3107

    Article  CAS  Google Scholar 

  • Men C, Liu RM, Xu F, Wang QR, Guo LJ, Shen ZY (2018) Pollution characteristics, risk assessment, and source apportionment of heavy metals in road dust in Beijing, China. Sci Total Environ 612:138–147

    Article  CAS  Google Scholar 

  • Min XY, Wu X, Shao PH, Ren Z, Ding L, Luo XB (2019) Ultra-high capacity of lanthanum-doped UiO-66 for phosphate capture: unusual doping of lanthanum by the reduction of coordination number. Chem Eng J 358:321–330

    Article  CAS  Google Scholar 

  • Mohamed F, Abukhadra MR, Shaban M (2018) Removal of safranin dye from water using polypyrrole nanofiber/Zn-Fe layered double hydroxide nanocomposite (Ppy NF/Zn-Fe LDH) of enhanced adsorption and photocatalytic properties. Sci Total Environ 640:352–363

    Article  Google Scholar 

  • Niu JR, Ding PJ, Jia XX, Hu GZ, Li ZX (2019) Study of the properties and mechanism of deep reduction and efficient adsorption of Cr(VI) by low-cost Fe3O4-modified ceramsite. Sci Total Environ 688:994–1004

    Article  CAS  Google Scholar 

  • Sahu S, Kar P, Bishoyi N, Mallik L, Patel RK (2019) Synthesis of polypyrrole-modified layered double hydroxides for efficient removal of Cr(VI). J Chem Eng Data 64:4357–4368

    Article  CAS  Google Scholar 

  • Sellami F, Kebiche-Senhadji O, Marais S, Colasse L, Fatyeyeva K (2020) Enhanced removal of Cr(VI) by polymer inclusion membrane based on poly (vinylidene fluoride) and Aliquat 336. Sep Purif Technol 248

  • Shao ZC, Huang C, Wu Q, Zhao Y, Xu W, Liu Y, Dang J, Hou H (2019) Ion exchange collaborating coordination substitution: more efficient Cr(VI) removal performance of a water-stable Cu-II-MOF material. J Hazard Mater 378

  • Shi SQ, Yang JK, Liang S, Li MY, Gan Q, Xiao KK, Hu JP (2018) Enhanced Cr(VI) removal from acidic solutions using biochar modified by Fe3O4@SiO2-NH2 particles. Sci Total Environ 628-629:499–508

    Article  CAS  Google Scholar 

  • Sun XM, Gao G, Yan DW, Feng CQ (2017) Synthesis and electrochemical properties of Fe3O4@MOF core-shell microspheres as an anode for lithium ion battery application. Appl Surf Sci 405:52–59

    Article  CAS  Google Scholar 

  • Venkateswarlu S, Lee D, Yoon M (2016) Bioinspired 2D-carbon flakes and Fe3O4 nanoparticles composite for arsenite removal. ACS Appl Mater Interfaces 8:23876–23885

    Article  CAS  Google Scholar 

  • Wang H et al (2015) Facile synthesis of polypyrrole decorated reduced graphene oxide-Fe3O4 magnetic composites and its application for the Cr(VI) removal. Chem Eng J 262:597–606

    Article  CAS  Google Scholar 

  • Wang YL et al (2019) Facile synthesis of acid-modified UiO-66 to enhance the removal of Cr (VI) from aqueous solutions. Sci Total Environ 682:118–127

    Article  CAS  Google Scholar 

  • Wang HY et al (2020) Synthesis of core-shell UiO-66-poly(m-phenylenediamine) composites for removal of hexavalent chromium. Environ Sci Pollut Res 27:4115–4126

    Article  CAS  Google Scholar 

  • Wang T, Zheng LW, Liu YH, Tang W, Fang T, Xing BS (2020) A novel ternary magnetic Fe3O4/g-C3N4/Carbon layer composite for efficient removal of Cr (VI): A combined approach using both batch experiments and theoretical calculation. Sci Total Environ 730:138928

    Article  CAS  Google Scholar 

  • Wei J, Tu C, Yuan G, Bi D, Xiao L, Theng BKG, Wang H, Ok YS (2019) Carbon-coated montmorillonite nanocomposite for the removal of chromium (VI) from aqueous solutions. J Hazard Mater 368:541–549

    Article  CAS  Google Scholar 

  • Xing JY, Shen Y, Dang WW, Yang B, Fu WC, Wang W, Bai B (2020) Fabrication of a photoelectric-sensitive imprinting polymer by PPy-cross-linked Gel/CS complex and its comprehensive treatment of Cr(VI). Polym Bull 77:869–882

    Article  CAS  Google Scholar 

  • Xu QH, Wang YL, Jin LQ, Wang Y, Qin MH (2017) Adsorption of Cu (II), Pb (II) and Cr (VI) from aqueous solutions using black wattle tannin-immobilized nanocellulose. J Hazard Mater 339:91–99

    Article  CAS  Google Scholar 

  • Xu YL, Chen JY, Chen R, Yu PL, Guo S, Wang XF (2019) Adsorption and reduction of chromium (VI) from aqueous solution using polypyrrole/calcium rectorite composite adsorbent. Water Res 160:148–157

    Article  CAS  Google Scholar 

  • Yang YQ, Chen N, Feng CP, Li M, Gao Y (2018) Chromium removal using a magnetic corncob biochar/polypyrrole composite by adsorption combined with reduction: Reaction pathway and contribution degree. Colloid Surface A 556:201–209

    Article  CAS  Google Scholar 

  • Yi YQ, Tu GQ, Zhao DY, Tsang PE, Fang ZQ (2019) Biomass waste components significantly influence the removal of Cr(VI) using magnetic biochar derived from four types of feedstocks and steel pickling waste liquor. Chem Eng J 360:212–220

    Article  CAS  Google Scholar 

  • Zhang JM, Zhai SR, Li S, Xiao ZY, Song Y, An QD, Tian G (2013) Pb(II) removal of Fe3O4@SiO2-NH2 core-shell nanomaterials prepared via a controllable sol-gel process. Chem Eng J 215:461–471

    Article  Google Scholar 

  • Zhang L, Luo HJ, Liu PP, Fang W, Geng JJ (2016) A novel modified graphene oxide/chitosan composite used as an adsorbent for Cr(VI) in aqueous solutions. Int J Biol Macromol 87:586–596

    Article  CAS  Google Scholar 

  • Zhang L et al (2018) One-step in situ synthesis of CdS/SnO2 heterostructure with excellent photocatalytic performance for Cr(VI) reduction and tetracycline degradation. Chem Eng J 352:863–875

    Article  CAS  Google Scholar 

  • Zhu KR, Chen CL, Xu H, Gao Y, Tan XL, Alsaedi A, Hayat T (2017) Cr(VI) reduction and immobilization by core-double-shell structured magnetic polydopamine@zeolitic idazolate frameworks-8 microspheres. Acs Sustain Chem Eng 5:6795–6802

Download references

Funding

The Guangzhou Science and Technology Project (grant number 201904010319) helped the collection of data, the Social Development Fund of Guangdong Province (grant number 2017A020216018) helped the analysis of data,Chongqing Science and Technology Commission of China (cstc2019jcyj-msxmX0647) and Science and Technology Research Program of Chongqing Municipal Education Commission China (KJQN201801324) and Foundation for High-level Talents of Chongqing University of Arts and Sciences (R2018CH11) helped the interpretation of the data.

Author information

Authors and Affiliations

  1. School of Environment and Energy, South China University of Technology, Guangzhou, 510006, People’s Republic of China

    Tingting Zhou, Qianwei Liang, Xin Zhou & HanJin Luo

  2. The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters of Ministry of Education, Guangzhou, 510006, People’s Republic of China

    Tingting Zhou, Xin Zhou & HanJin Luo

  3. School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510641, People’s Republic of China

    Qianwei Liang

  4. Guangdong Engineering and Technology Research Center for Environmental Nanomaterials, Guangzhou, 510006, People’s Republic of China

    HanJin Luo

  5. Chongqing Key Laboratory of Environmental Materials & Remediation Technologies, Chongqing University of Art and Science, Chongqing, 402160, People’s Republic of China

    Wei Chen

Authors
  1. Tingting Zhou
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Qianwei Liang
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Xin Zhou
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. HanJin Luo
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Wei Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

TTZ contributed to the conception of the study, performed the experiment, contributed significantly to analysis and manuscript preparation, and performed the data analyses and wrote the manuscript; QWL, XZ, HJL, and WC helped perform the analysis with constructive discussions. All authors read and approved the final manuscript.

Corresponding author

Correspondence to HanJin Luo.

Ethics declarations

Competing interests

The authors declare that they have no competing interests.

Additional information

Responsible Editor: Tito Roberto Cadaval Jr

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

Zhou, T., Liang, Q., Zhou, X. et al. Enhanced removal of toxic hexavalent chromium from aqueous solution by magnetic Zr-MOF@polypyrrole: performance and mechanism. Environ Sci Pollut Res 28, 13084–13096 (2021). https://doi.org/10.1007/s11356-021-12341-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-021-12341-x

Keywords

Search

Navigation