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Ethylenediaminetetraacetic acid intercalated MgAl-layered double-hydroxides nanocomposite as an efficient platform in the development of electrochemical sensor for the detection of iron (II)

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Abstract

The significance of iron in maintaining physiological homeostasis in the human body is well recognized. However, the presence of unbound iron, specifically the non-transferrin bound iron (NTBI), can potentially induce tissue damage in crucial organs, such as the heart, kidney, and liver. Consequently, there arises a critical need to establish a sensing platform with the capability of detecting exceedingly low concentrations of iron (II). To address this imperative, a layered double-hydroxide (LDH) structure comprising Mg2+ and Al3+ with ethylenediaminetetraacetic acid (EDTA) intercalated between the layers has been successfully synthesized. The proposed methodology involves the utilization of a differential pulse voltammetric detection approach to identify Fe2+ on an EDTA-MgAl LDHs composite-modified glassy carbon electrode. Scanning Electron Microscopy (SEM) analysis of the EDTA-MgAl LDHs revealed the stratified structure of sheets with thicknesses ranging from 95 to 160 nm. Voltammetry studies further demonstrated the effective Fe2+ capturing ability of EDTA and confirmed the existence of multi-layered MgAl LDHs, which contribute to the electrocatalytic oxidation of Fe2+ to Fe3+. The developed sensor exhibited an elevated sensitivity (0.061 µA µM−1) towards Fe2+ and a wide linear detection ranges from 0.1 to 102.1 µM, with an exceptionally low detection limit of 50 nM. Furthermore, the applicability of a two-segmented piecewise linear function to estimate the breakpoint Fe2+ concentration, above and below which the sensor's response behaviour changes, was assessed for the direct determination of Fe2+ in a 0.1 M KCl solution. In conclusion, the developed sensor possesses several advantageous attributes, including a rapid response time, effective Fe2+ capturing ability, electrocatalytic capability, wide linearity, and resistance to interference from other metal ions. These characteristics collectively render it a highly promising and efficient sensing platform for diverse Fe2+ detection applications.

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References

  1. Speich M, Pineau A, Ballereau F (2001) Minerals, trace elements and related biological variables in athletes and during physical activity. Clin Chim Acta 312:1–11. https://doi.org/10.1016/S0009-8981(01)00598-8

    Article  CAS  PubMed  Google Scholar 

  2. Patel M, Ramavataram DVSS (2012) Non transferrin bound iron: nature, manifestations and analytical approaches for estimation. Indian J Clin Biochem 27:322–332. https://doi.org/10.1007/s12291-012-0250-7

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  3. Hershko C, Graham G, Bates GW, Rachmilewitz EA (1978) Non-specific serum iron in thalassaemia: an abnormal serum iron fraction of potential toxicity. Br J Haematol 40:255–263. https://doi.org/10.1111/j.1365-2141.1978.tb03662.x

    Article  CAS  PubMed  Google Scholar 

  4. Gutteridge JM, Rowley DA, Halliwell B (1981) Superoxide-dependent formation of hydroxyl radicals in the presence of iron salts. Detection of “free” iron in biological systems by using bleomycin-dependent degradation of DNA. Biochem J 199:263–265. https://doi.org/10.1042/bj1990263

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  5. Matta MK, Beekman CR, Gandhi A et al (2018) Determination of non-transferrin bound iron, transferrin bound iron drug bound iron and total iron in serum in a rats after IV administration of sodium ferric gluconate complex by simple ultrafiltration inductively coupled plasma mass spectrometric dete. Nanomater (Basel, Switzerland). https://doi.org/10.3390/nano8020101

    Article  Google Scholar 

  6. Merli D, Profumo A, Dossi C (2012) An analytical method for Fe(II) and Fe(III) determination in pharmaceutical grade iron sucrose complex and sodium ferric gluconate complex. J Pharm Anal 2:450–453. https://doi.org/10.1016/j.jpha.2012.05.003

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  7. Mahmoud WH (2001) Iron ion-selective electrodes for direct potentiometry and potentiotitrimetry in pharmaceuticals. Anal Chim Acta 436:199–206. https://doi.org/10.1016/S0003-2670(01)00892-3

    Article  CAS  Google Scholar 

  8. Aghaie M, Giahi M, Aghaie H et al (2009) New Fe(II) Ion-selective electrode based on N-phenylaza-15-crown-5 as neutral carrier in PVC matrix. Desalination 247:346–354. https://doi.org/10.1016/j.desal.2008.10.007

    Article  CAS  Google Scholar 

  9. Yazdely M, Taher MA, Tajik S (2013) PVC membrane potentiometric sensor based on (E)-2-acetyl-3-(butyl-amino)-N-phenyl buten-2-thioamide for selective determination of iron(II). Anal Bioanal Electrochem 5:467–480

    CAS  Google Scholar 

  10. Kumar S, Mittal S, Kaur N, Kaur R (2017) Improved performance of Schiff based ionophore modified with MWCNT for Fe( ii ) sensing by potentiometry and voltammetry supported with DFT studies. RSC Adv 7:16474–16483

    Article  CAS  Google Scholar 

  11. Absalan G, Arabi M, Khalifeh R et al (2014) Coated wire ion selective electrode based on a new crown ether for determination of ${\rm Fe}^{2+}$. IEEE Sens J 14:349–356. https://doi.org/10.1109/JSEN.2013.2282320

    Article  CAS  Google Scholar 

  12. Pérez MR, Pavlovic I, Barriga C et al (2006) Uptake of Cu2+, Cd2+ and Pb2+ on Zn–Al layered double hydroxide intercalated with edta. Appl Clay Sci 32:245–251. https://doi.org/10.1016/j.clay.2006.01.008

    Article  CAS  Google Scholar 

  13. Zhao D, Sheng G, Hu J et al (2011) The adsorption of Pb(II) on Mg2Al layered double hydroxide. Chem Eng J 171:167–174. https://doi.org/10.1016/j.cej.2011.03.082

    Article  CAS  Google Scholar 

  14. Mohamed MEB, Attia NF, Elashery SEA (2021) Greener and facile synthesis of hybrid nanocomposite for ultrasensitive iron (II) detection using carbon sensor. Microporous Mesoporous Mater 313:110832. https://doi.org/10.1016/j.micromeso.2020.110832

    Article  CAS  Google Scholar 

  15. Stozhko N, Morosanova E, Kolyadina L, Azarova Z (2004) An electrochemical sol–gel sensor for determining iron by stripping voltammetry. J Anal Chem—J Anal Chem-Engl TR 59:865–870. https://doi.org/10.1023/B:JANC.0000040702.79361.bc

    Article  CAS  Google Scholar 

  16. Abounassif MA, Al-Omar MA, Amr A-GE, Mostafa GAE (2011) PVC membrane sensor for potentiometric determination of iron (II) in some pharmaceutical formulations based on a new neutral ionophore. Drug Test Anal 3:373–379. https://doi.org/10.1002/dta.231

    Article  CAS  PubMed  Google Scholar 

  17. Farahani N, Aghaie H (2008) Fe (II) ion-selective membrane electrode based ontetra-phenyl porphyrin in PVC matrix. J Phys Theor Chem 5:17–22

    Google Scholar 

  18. Kamal A, Kumar N, Bhalla V et al (2014) Rhodamine-dimethyliminocinnamyl based electrochemical sensors for selective detection of iron (II). Sensors Actuators B Chem 190:127–133. https://doi.org/10.1016/j.snb.2013.08.079

    Article  CAS  Google Scholar 

  19. Aglan RF, Rizk MS, Mohamed GG, El-Wahy AH, Mohamed HA (2014) Preparation and properties of a new carbon paste iron selective electrodes and their applications. Am J Anal Chem 5:140–148. https://doi.org/10.4236/ajac.2014.52017

    Article  CAS  Google Scholar 

  20. Frag EY, Abd El-Ghany NA, Fattah MAEL (2018) Physico-chemical properties and characterization of iron (II) electrochemical sensor based on carbon paste electrode modified with novel antimicrobial carboxymethyl chitosan-graft-poly(1-cyanoethanoyl-4-acryloyl-thiosemcarbazide) copolymers. J Electroanal Chem 808:266–277. https://doi.org/10.1016/j.jelechem.2017.12.018

    Article  CAS  Google Scholar 

  21. Norocel L, Gutt G (2019) Development and performance testing of an electrochemical sensor for determination of iron ions in wine. Aust J Grape Wine Res 25:161–164. https://doi.org/10.1111/ajgw.12375

    Article  CAS  Google Scholar 

  22. Sreekumar A, Durai L, Badhulika S (2023) Facile one-step synthesis of a niobium iron oxide based electrochemical transistor for rapid{,} label-free detection of folic acid in human blood serum samples. New J Chem 47:8845–8853. https://doi.org/10.1039/D3NJ00475A

    Article  CAS  Google Scholar 

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Acknowledgements

The research was supported by Professor T. R. Rajagopalan research fund, SASTRA Deemed University. The authors are grateful to Department of Science and Technology, New Delhi (SR/FST/ET-I/2018/221(c)) for the financial support. We acknowledge SASTRA Deemed to be University, Thanjavur for extending infrastructure support to carry out the study.

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Shruthee Sankarlinkam—investigation, methodology, conceptualization, data curation, writing original draft, Indhu Suresh—investigation, methodology, conceptualization, writing original draft, G. Hariharan—mathematical analysis, review and editing, Noel Nesakumar—formal analysis, data curation, writing review & editing, Arockia Jayalatha Kulandaisamy—formal analysis, data curation, original draft, John Bosco Balaguru Rayappan—formal analysis, project administration, funding acquisition, and writing review & editing. All authors participated in the discussion, contributing to the final manuscript.

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Correspondence to John Bosco Balaguru Rayappan.

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Sankarlinkam, S., Suresh, I., Hariharan, G. et al. Ethylenediaminetetraacetic acid intercalated MgAl-layered double-hydroxides nanocomposite as an efficient platform in the development of electrochemical sensor for the detection of iron (II). J Appl Electrochem 54, 309–321 (2024). https://doi.org/10.1007/s10800-023-01970-4

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