Abstract
The effects of aging of colloidal dispersions of iron (oxyhydr)oxides affect the stability of these materials under different environmental conditions, thereby affecting their reactivity and applicability in remediation. However, only a limited number of studies have focused on aging-induced changes in the phase composition, surface properties, and toxicological effects of nanoparticles (NPs). In this study, closely related and intermediate iron (oxyhydr)oxides (Fe3-δO4, γ-Fe2O3, 5Fe2O3∙9H2O, δ-FeOOH) were synthesized. The crystal structure, surface charge, and leaching of Fe ions of these materials were analyzed. All synthesized materials were then tested in bioassays with ciliates and higher plants at circumneutral pH, both upon preparation and after aqueous aging. Quantitative analysis of the X-ray diffraction data using the Rietveld method showed that the crystal structure of the magnetite NPs changed to γ-Fe2O3. The evaluation of biological activity in Sinapis alba (white mustard) showed that NPs of different compositions, stored at a maximum concentration of 10 g L−1, inhibited root growth by 50%. In the case of δ-FeOOH and Fe3O4, however, concentrations of 1 g L−1 caused only minor inhibition. The toxic effects of Fe-NPs, attributed to the release of Fe2+ and Fe3+ ions by oxidation, were found to be consistent with the redox behavior of NPs.
Similar content being viewed by others
References
Anjum M, Miandad R, Waqas M, Gehany F, Barakat MA (2019) Remediation of wastewater using various nano-materials. Arabian J Chem 12:4897–4919. https://doi.org/10.1016/j.arabjc.2016.10.004
Auffan M, Achouak W, Rose J, Roncato MA, Chanéac C, Waite DT, Masion JYA, Woicik JC, Wiesner MR, Bottero JY (2008) Relation between the redox state of iron-based nanoparticles and their cytotoxicity toward Escherichia coli. Environ Sci Technol 42:6730–6735. https://doi.org/10.1021/es800086f
Baalousha M (2009) Aggregation and disaggregation of iron oxide nanoparticles: influence of particle concentration, pH and natural organic matter. Sci Total Environ 407(6):2093–2101. https://doi.org/10.1016/j.scitotenv.2008.11.022
Baragaño D, Alonso J, Gallego JR, Lobo MC, Gil-Díaz M (2020) Magnetite nanoparticles for the remediation of soils co-contaminated with As and PAHs. Chem Eng J 399:125809. https://doi.org/10.1016/j.cej.2020.125809
Bogart LK, Blanco-Andujar C, Pankhurst QA (2018) Environmental oxidative aging of iron oxide nanoparticles. Appl Phys Lett 113:133701. https://doi.org/10.1063/1.5050217
Bondarenko L, Kahru A, Terekhova V, Dzhardimalieva G, Uchanov P, Kydralieva K (2020a) Effects of humic acids on the ecotoxicity of Fe3O4 nanoparticles and Fe-Ions: impact of oxidation and aging. Nanomaterials 10:1–18. https://doi.org/10.3390/nano10102011
Bondarenko LS, Kovel ES, Kydralieva KA, Dzhardimalieva GI, Illés E, Tombácz E, Kicheeva AG, Kudryasheva NS (2020b) Effects of modified magnetite nanoparticles on bacterial cells and enzyme reactions. Nanomaterials 10:1499. https://doi.org/10.3390/nano10081499
Bondarenko L, Pankratov D, Dzeranov A et al (2022) A simple method for the quantification nonstoichiometric magnetite using conventional X-ray diffraction technique. Mendeleev Commun 32:642–644. https://doi.org/10.1016/j.mencom.2022.09.025
Chen PJ, Tan SW, Wu W-L (2012) Stabilization or oxidation of nanoscale zerovalent iron at environmentally relevant exposure changes bioavailability and toxicity in medaka fish. Environ Sci Technol 46(15):8431–8439. https://doi.org/10.1021/es3006783
Cornell RM, Schwertmann U (2003) The iron oxides: structure, properties, reactions, occurrences and uses. Wiley-VCH, Weinheim
Das S, Hendry MJ, Essilfie-Dughan J (2011) Transformation of two-line ferrihydrite to goethite and hematite as a function of pH and temperature. Environ Sci Technol 45(1):268–275. https://doi.org/10.1021/es101903y
Devatha CP, Shivani S (2020) Novel application of maghemite nanoparticles coated bacteria for the removal of cadmium from aqueous solution. J Environ Manag 258:110038. https://doi.org/10.1016/j.jenvman.2019.110038
Dogra R, Roverso M, Di Bernardo G, Zanut A, Monikh FA, Pettenuzzo S, Pastore P, Bogialli S (2023) Metallic functionalization of magnetic nanoparticles enhances the selective removal of glyphosate, AMPA, and glufosinate from surface water. Environ Sci: Nano 10:2399–2411. https://doi.org/10.1039/D3EN00129F
Dzeranov A, Bondarenko L, Pankratov D, Prokof‘ev M, Dzhardimalieva G, Jorobekova S, Tropskaya N, Telegina L, Kydralieva K (2022) Iron oxides nanoparticles as components of ferroptosis-inducing systems: screening of potential candidates. Magnetochemistry 9(1):3. https://doi.org/10.3390/magnetochemistry9010003
Dzeranov A, Bondarenko L, Pankratov D et al (2023) Impact of silica-modification and oxidation on crystal structure of magnetite. Magnetochemistry 9:18. https://doi.org/10.3390/magnetochemistry9010018
Elmore WC (1938) Ferromagnetic colloid for studying magnetic structures. Phys Rev 54(4):309–310. https://doi.org/10.1103/physrev.54.309
COMMISSION DIRECTIVE 93/67/EEC of 20 July 1993 laying down the principles (or assessment of risks to man and the environment of substances notified in accordance with Council Directive 67/548/EEC. Official Journal of the European Communities. Directives originating from the EU 1993 No. 67, 8.9.93, No L 227/9-18
Fan J, Zhao Z, Ding Z, Liu J (2018) Synthesis of different crystallographic FeOOH catalysts for peroxymonosulfate activation towards organic matter degradation. RSC Adv 8(13):7269–7279. https://doi.org/10.1039/c7ra12615h
Gorski CA, Scherer MM (2010) Determination of nanoparticulate magnetite stoichiometry by mossbauer spectroscopy, acidic dissolution, and powder X-Ray diffraction: a critical review. Am Mineral 95:1017–1026. https://doi.org/10.2138/am.2010.3435
Gubler R, Laurel K, Arrigo T (2021) Ferrous iron enhances arsenic sorption and oxidation by non-stoichiometric magnetite and maghemite. J Hazard Mater 402:123425. https://doi.org/10.1016/j.jhazmat.2020.123425
Guerra FD, Attia MF, Whitehead DC, Alexis F (2018) Nanotechnology for environmental remediation: materials and applications. Molecular 23:1760. https://doi.org/10.3390/molecules23071760
Guivar J, Martínez A, Anaya A, Valladares L, Félix L, Dominguez A (2014) Structural and magnetic properties of monophasic maghemite (γ-Fe2O3) nanocrystalline. Powder ANP 3:114–121. https://doi.org/10.4236/anp.2014.33016
Handler RM, Beard BL, Johnson CM et al (2009) Atom exchange between aqueous Fe(II) and Goethite: an Fe isotope tracer study. Environ Sci Technol 43:1102–1107. https://doi.org/10.1021/es802402m
Horst MF, Lassalle V, Ferreira ML (2015) Nanosized magnetite in low cost materials for remediation of water polluted with toxic metals, azo- and antraquinonic dyes. Front Environ Sci Eng 9:746–769. https://doi.org/10.1007/s11783-015-0814-x
Hu J, Chen G, Lo IMC (2005) Removal and recovery of Cr(VI) from wastewater by maghemite nanoparticles. Water Res 39:4528–4536. https://doi.org/10.1016/j.watres.2005.05.051
Jambor JL, Dutrizac JE (1998) Occurrence and constitution of natural and synthetic ferrihydrite, a widespread iron oxyhydroxide. Chem Rev 98:2549–2586. https://doi.org/10.1021/cr970105t
Jaydeep MB, Himanshu PK, Mousumi C (2022) Adsorption of hexavalent chromium from aqueous stream by maghemite nanoparticles synthesized by the microemulsion method. Energy Nexus 5:100035. https://doi.org/10.1016/j.nexus.2021.100035
Jeon S, Clavadetscher J, Lee D-K et al (2018) Surface charge-dependent cellular uptake of polystyrene nanoparticles. Nanomaterials 8:1028. https://doi.org/10.3390/nano8121028
Jungcharoen P, Pédrot M, Choueikani F, Pasturel M, Hanna K, Heberling F, Tesfa M, Marsac R (2021) Probing the effects of redox conditions and dissolved Fe2+ on nanomagnetite stoichiometry by wet chemistry, XRD, XAS and XMCD. Environ Sci Nano 8:2098–2107. https://doi.org/10.1039/D1EN00219H
Jungcharoen P, Pédrot M, Heberling F, Hanna K, Choueikani F, Catrouillet C, Dia A, Marsac R (2022) Prediction of nanomagnetite stoichiometry (Fe(ii)/Fe(iii)) under contrasting pH and redox conditions. Environ Sci Nano 9:2363–2371. https://doi.org/10.1039/D2EN00112H
Kicheeva A, Sushko E, Bondarenko L et al (2023) Functionalized magnetite nanoparticles: characterization, bioeffects, and role of reactive oxygen species in unicellular and enzymatic systems. Int J Mol Sci 24:1133. https://doi.org/10.3390/ijms24021133
Kim W, Suh CY, Cho SW, Roh KM, Kwon H, Song K, Shon IJ (2012) A new method for the identification and quantification of magnetite–maghemite mixture using conventional X-ray diffraction technique. Talanta 94:348–352. https://doi.org/10.1016/j.talanta.2012.03.001
Kim JH, Lee Y, Kim EJ, Gu S, Sohn EJ, Seo YS, An HJ, Chang YS (2014) Exposure of iron nanoparticles to arabidopsis thaliana enhances root elongation by triggering cell wall loosening. Environ Sci Technol 48:3477–3485. https://doi.org/10.1021/es4043462
Kydralieva KA, Dzhardimalieva GI, Yurishcheva AA, Jorobekova SJ (2016) Nanoparticles of magnetite in polymer matrices: synthesis and properties. J Inorg Organomet Polym Mater 26:1212–1230. https://doi.org/10.1007/s10904-016-0436-1
Lei C, Sun Y, Tsang DCW, Lin D (2018) Environmental transformations and ecological effects of iron-based nanoparticles. Environ Pollut 232:10–30. https://doi.org/10.1016/j.envpol.2017.09.052
Liang C, Fu F, Tang B (2021) Mn-incorporated ferrihydrite for Cr(VI) immobilization: adsorption behavior and the fate of Cr(VI) during aging. J Hazard Mater 417:126073. https://doi.org/10.1016/j.jhazmat.2021.126073
Lindsley DH (1991) Experimental studies of oxide minerals. Rev Mineral Geochem 25:69–106
Liu Y, Li W, Lao F et al (2011) Intracellular dynamics of cationic and anionic polystyrene nanoparticles without direct interaction with mitotic spindle and chromosomes. Biomaterials 32:8291–8303. https://doi.org/10.1016/j.biomaterials.2011.07.037
Liu G, Gao J, Ai H, Chen X (2013a) Applications and potential toxicity of magnetic iron oxide nanoparticles. Small 9:1533–1545. https://doi.org/10.1002/smll.201201531
Liu T, Li X, Waite TD (2013b) Depassivation of aged Fe0 by ferrous ions: implications to contaminant degradation. Environ Sci Technol 47:13712–13720. https://doi.org/10.1021/es403709v
Liu CH, Chuang YH, Chen TY, Tian Y, Li H, Wang MK, Zhang W (2015) Mechanism of arsenic adsorption on magnetite nanoparticles from water: thermodynamic and spectroscopic studies. Environ Sci Technol 49:7726–7734. https://doi.org/10.1021/acs.est.5b00381
Lu B, Guo H, Li P, Liu H, Wei Y, Hou D (2011) Comparison study on transformation of iron oxyhydroxides: based on theoretical and experimental data. J Solid State Chem 184:2139–2144. https://doi.org/10.1016/j.jssc.2011.06.008
Ma X, Gurung A, Deng Y (2013) Phytotoxicity and uptake of nanoscale zero-valent iron (nZVI) by two plant species. Sci Total Environ 443:844–849. https://doi.org/10.1016/j.scitotenv.2012.11.073
Maity D, Agrawal DC (2007) Synthesis of iron oxide nanoparticles under oxidizing environment and their stabilization in aqueous and non-aqueous media. J Magn Magn Mater 308:46–55. https://doi.org/10.1016/j.jmmm.2006.05.001
Makhlouf SA, Parker FT, Berkowitz AE (1997) Magnetic hysteresis anomalies in ferritin. Phys Rev B 55:14717. https://doi.org/10.1103/PhysRevB.55.R14717
Moons N, Slaveykova VI (2014) Oxidative stress induced by inorganic nanoparticles in bacteria and aquatic microalgae–state of the art and knowledge gaps. Nanotoxicology 8:605–630. https://doi.org/10.3109/17435390.2013.809810
Mulens-Arias V, Rojas JM, Barber DF (2020) The intrinsic biological identities of iron oxide nanoparticles and their coatings: unexplored territory for combinatorial therapies. Nanomaterials 10:837. https://doi.org/10.3390/nano10050837
Narwal N, Katyal D, Navish K, Pawan KR, Sudhir GW, Arivalagan P, Ghotekar S, Kuan SK (2023) Emerging micropollutants in aquatic ecosystems and nanotechnology-based removal alternatives: a review. Chemosphere 341:139945. https://doi.org/10.1016/j.chemosphere.2023.139945
Ngomsik A-F, Bee A, Talbot D, Cote G (2012) Magnetic solid–liquid extraction of Eu(III), La(III), Ni(II) and Co(II) with maghemite nanoparticles. Sep Purif Technol 86:1–8. https://doi.org/10.1016/j.seppur.2011.10.013
Nikolaeva OV, Terekhova VA (2017) Improvement of laboratory phytotest for the ecological evaluation of soils. Eurasian Soil Sci 50:1105. https://doi.org/10.1134/S1064229317090058
Nikolic D, Panjan M, Blake GR, Tadic M (2015) Annealing-dependent structural and magnetic properties of nickel oxide (NiO) nanoparticles in a silica matrix. J Eur Ceram Soc 35:3843–3852. https://doi.org/10.1016/j.jeurceramsoc.2015.06.024
Notter DA, Mitrano DM, Nowack B (2014) Are nanosized or dissolved metals more toxic in the environment? A meta-analysis. Environ Toxicol Chem 33:2733–2739. https://doi.org/10.1002/etc.2732
Pinto ISX, Pacheco PHVV, Coelho JV, Lorencon E, Ardisson JD, Fabris JD, De Souza PP, Krambrock KWH, Oliveira LC, Pereira MC (2012) Nanostructured δ-FeOOH: an efficient Fenton-like catalyst for the oxidation of organics in water. Appl Catal B: Environ 119:175–182. https://doi.org/10.1016/j.apcatb.2012.02.026
Poulton SW, Canfield DE (2005) Development of a sequential extraction procedure for iron: Implications for iron partitioning in continentally derived particulates. Chem Geol 214:209–221. https://doi.org/10.1016/j.chemgeo.2004.09.003
Qadri S, Ganoe A, Haik Y (2009) Removal and recovery of acridine orange from solutions by use of magnetic nanoparticles. J Hazard Mater 169:318–323. https://doi.org/10.1016/j.jhazmat.2009.03.103
Rajput S, Singh LP, Pittman CU, Mohan D (2017) Lead (Pb2+) and copper (Cu2+) remediation from water using superparamagnetic maghemite (γ-Fe2O3) nanoparticles synthesized by Flame Spray Pyrolysis (FSP). J Coll Int Sci 492:176–190. https://doi.org/10.1016/j.jcis.2016.11.095
Salari M, Rakhshandehroo GR, Nikoo MR, Zerafat MM, Mooselu MG (2021) Optimal degradation of ciprofloxacin in a heterogeneous Fenton-like process using (δ-FeOOH)/MWCNTs nanocomposite. Environ Technol Innov 23:101625. https://doi.org/10.1016/j.eti.2021.101625
Sangaiya P, Jayaprakash RA (2018) A review on iron oxide nanoparticles and their biomedical applications. J Supercond Nov Magn 31:3397–3413. https://doi.org/10.1007/s10948-018-4841-2
Schaeublin NM, Braydich-Stolle LK, Schrand AM et al (2011) Surface charge of gold nanoparticles mediates mechanism of toxicity. Nanoscale 3:410–420. https://doi.org/10.1039/c0nr00478b
Scherer MM, Balko BA, Tratnyek PG (1999) The role of oxides in reduction reactions at the metal-water interface. Mineral-water interfacial reactions. In: Sparks DL, Grundl TJ (eds), ACS symposium series 715, American chemical society, Washington, DC, pp 301–322
Schwaminger SP, Bauer D, Fraga-García P, Wagner FE, Berensmeier S (2017) Oxidation of magnetite nanoparticles: impact on surface and crystal properties. Cryst Eng Comm 19:246–255. https://doi.org/10.1039/C6CE02421A
Sharifi HD, Ksenofontov V, Moller A, Jakob G, Asadi K (2018) Determining magnetite/maghemite composition and core-shell nanostructure from magnetization curve for iron oxide nanoparticles. J Phys Chem 122:28292–28301. https://doi.org/10.1021/acs.jpcc.8b06927
Shi J, Zhang J, Wang C, Liu Y, Li J (2023) Research progress on the magnetite nanoparticles in the fields of water pollution control and detection. Chemosphere 336:139220. https://doi.org/10.1016/j.chemosphere.2023.139220
Smržová D, Ramteke PM, Ecorchard P, Šubrt J, Bezdička P, Kubániová D, Kormunda M, Maršálek R, Vislocká X, Vykydalová A, Singh SK, Wathore R, Shinde VM, Labhasetwar NK (2023) Simultaneous removal of selenium and microbial contamination from drinking water using modified ferrihydrite-based adsorbent. J Water Process Eng 56:104337. https://doi.org/10.1016/j.jwpe.2023.104337
Sun ZX, Su FW, Forsling W, Samskog PO (1998) Surface characteristics of magnetite in aqueous suspension. J Colloid Interface Sci 197:151–159. https://doi.org/10.1006/jcis.1997.5239
Sun Y, Ma M, Zhang Y, Gu N (2004) Synthesis of nanometer-size maghemite particles from magnetite. Colloids Surf A Physicochem Eng Asp 245:15–19. https://doi.org/10.1016/j.colsurfa.2004.05.009
Sundman A, Byrne JM, Bauer I, Menguy N, Kappler A (2017) Interactions between magnetite and humic substances: redox reactions and dissolution processes. Geochem Trans 18(1):6–15. https://doi.org/10.1186/s12932-017-0044-1
Tao Z, Zhou Q, Zheng T, Mo F, Ouyang S (2023) Iron oxide nanoparticles in the soil environment: adsorption, transformation, and environmental risk. J Hazard Mater 45:132107. https://doi.org/10.1016/j.jhazmat.2023.132107
Taylor RM, Schwertmann E (1974) Maghemite in soils and its origin. I. Properties and observations on soil maghemites. Clay Miner 10:289–298
Toby BH (2006) R factors in rietveld analysis: how good is good enough. Powder Diffr 21:67–70. https://doi.org/10.1154/1.2179804
Tombácz E, Illés E, Majzik A, Hajdú A, Rideg N, Szekeres M (2007) Ageing in the inorganic nanoworld: example of magnetite nanoparticles in aqueous medium. Croat Chem Acta 80:503–515
Untener EA, Comfort KK, Maurer EI et al (2013) Tannic acid coated gold nanorods demonstrate a distinctive form of endosomal uptake and unique distribution within cells. ACS Appl Mater Interfaces 5:8366–8373. https://doi.org/10.1021/am402848q
Usman M, Byrne JM, Chaudhary A, Orsetti S, Hanna K, Ruby C, Kappler A, Haderlein SB (2018) Magnetite and green rust: synthesis, properties, and environmental applications of mixed-valent iron minerals. Chem Rev 118:3251–3304. https://doi.org/10.1021/acs.chemrev.7b00224
Wang J, Sun J, Sun Q, Chen Q (2003) One-step hydrothermal process to prepare highly crystalline Fe3O4 nanoparticles with improved magnetic properties. Mater Res Bull 38:1113–1118. https://doi.org/10.1016/S0025-5408(03)00129-6
Wang Y, Fang J, Crittenden JC, Shen C (2017) Novel RGO/α-FeOOH supported catalyst for Fenton oxidation of phenol at a wide pH range using solar-light-driven irradiation. J Hazard Mater 329:321–329. https://doi.org/10.1016/j.jhazmat.2017.01.041
Wu S, Lu J, Ding Z, Li N, Fu F, Tang B (2016) Cr (VI) removal by mesoporous FeOOH polymorphs: performance and mechanism. RSC Adv 6:82118–82130. https://doi.org/10.1039/C6RA14522A
Yadav VK, Fulekar MH (2018) Biogenic synthesis of maghemite nanoparticles (γ-Fe2O3) using tridax leaf extract and its application for removal of fly ash heavy metals (Pb, Cd). Mater Proc 5:20704–20710. https://doi.org/10.1016/j.matpr.2018.06.454
Yuan K, Ilton ES, Antonio MR et al (2015) Electrochemical and spectroscopic evidence on the one-electron reduction of U (VI) to U (V) on magnetite. Environ Sci Technol 49:6206–6213. https://doi.org/10.1021/acs.est.5b00025
Yuan K, Lee SS, Cha W, Ulvestad A, Kim H, Abdilla B, Sturchio NC, Fenter P (2019) Oxidation induced strain and defects in magnetite crystals. Nat Commun 10:703. https://doi.org/10.1038/s41467-019-08470-0
Zhang P, Liu A, Huang P, Min L, Sun H (2020a) Sorption and molecular fractionation of biochar-derived dissolved organic matter on ferrihydrite. J Hazard Mater 392:122260. https://doi.org/10.1016/j.jhazmat.2020.122260
Zhang S, Du Q, Sun Y et al (2020b) Fabrication of L-cysteine stabilized α-FeOOH nanocomposite on porous hydrophilic biochar as an effective adsorbent for Pb2+ removal. Sci Total Environ 720:137415. https://doi.org/10.1016/j.scitotenv.2020.137415
Zhang Y, Li H, Jiang Q, Jiang S, Wang Y, Wang L (2021) One-pot synthesis of a novel P-doped ferrihydrite nanoparticles for efficient removal of Pb (II) from aqueous solutions: performance and mechanism. J Environ Chem Eng 9:105721. https://doi.org/10.1016/j.jece.2021.105721
Acknowledgements
This research was supported by the Russian Science Foundation (project No 23-23-00621).
Author information
Authors and Affiliations
Corresponding author
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Dzeranov, A., Bondarenko, L., Saman, D. et al. Effects of water-induced aging on iron (oxyhydr)oxides nanoparticles: linking crystal structure, iron ion release, and toxicity. Chem. Pap. 78, 4029–4043 (2024). https://doi.org/10.1007/s11696-024-03373-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11696-024-03373-x