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Immobilizing arsenic in soil via amine metal complex: a case study using iron-ethylenediamine

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Abstract

Fe-based nanomaterials have been extensively investigated for their application in mitigating arsenic (As) pollution in groundwater, sediment, and soils. Here, an iron-ethylenediamine (Fe-EDA) complex was synthesized and characterized using Fourier transform-infrared spectroscopy and X-ray photoelectron spectroscopy before its use as an amendment to ameliorate As-polluted soils. Column leaching tests at three Fe-EDA application rates (1%, 3%, and 5%) were conducted, and their results were compared with those acquired after using nano zerovalent iron (nZVI) and Fe3O4, to assess their efficiency to amend As-contaminated paddy soils. After leaching, stabilization efficiency and soil chemical characteristics were determined. Additionally, As fractions were measured using inductively coupled plasma–mass spectroscopy by employing a sequential extraction procedure to evaluate the performance of the treatments and understand the underlying their mechanisms. Compared with the control treatment, the Fe-EDA treatment reduced As release by more than 35.33% in the 2nd leaching cycle, whereas nZVI and Fe3O4 decreased the As release by 11.84% and 24.60%, respectively. Moreover, the optimal addition of the Fe-EDA chelate was 5%, which stabilized more than 50% As in the soil from the 7th to 11th leaching cycles. After sequential extraction, the Fe–Mn oxide binding fraction, which was originally 12.65%, increased to 21.5%, 18.23%, and 21.71% after the application of nZVI, Fe3O4, and Fe-EDA amendments, respectively. Furthermore, our treatments promoted the binding of the As fraction with crystalline Fe (III) (oxyhydr)oxide (F3); however, other fractions did not increase considerably, suggesting that the Fe-EDA complex could effectively stabilize As through electrostatic attraction between the arsenate anion and EDA, as well as As-O-Fe bond formation via a coordinating reaction. Overall, Fe-EDA was found to be a potent amendment for mitigating As-polluted soil.

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References

  • Ahmadijokani F, Tajahmadi S, Bahi A, Molavi H, Rezakazemi M, Ko F, Aminabhavi TM, Arjmand M (2021) Ethylenediamine-functionalized Zr-based MOF for efficient removal of heavy metal ions from water. Chemosphere 264:128466–128474

    CAS  Google Scholar 

  • Akoto JD, Chai F, Repo E, Yang Z, Wang D, Zhao F, Liao Q, Chai L (2022) Polyethyleneimine stabilized nanoscale zero-valent iron-magnetite (Fe3O4@nZVI-PEI) for the enhanced removal of arsenic from acidic aqueous solution: performance and mechanisms. J Environ Chem Eng 10(6):108589. https://doi.org/10.1016/j.jece.2022.108589

  • Baragano D, Alonso J, Gallego JR, Lobo MC, Gil-Diaz M (2020) Zero valent iron and goethite nanoparticles as new promising remediation techniques for As-polluted soils. Chemosphere 238:124624–124633

    CAS  Google Scholar 

  • 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 399:125809–125818

    Google Scholar 

  • Barreto MSC, Elzinga EJ, Alleoni LRF (2020) Hausmannite as potential As(V) filter. Macroscopic and spectroscopic study of As(V) adsorption and desorption by citric acid. Environ Pollut 262:114196

    CAS  Google Scholar 

  • Cao Y, Zhang B, Guo M, Wang X, Zhu Y (2022) Long-term stabilization of lead contaminated soil with a novel dithiocarboxylate functionalized hyperbranched polymer. J Environ Chem Eng 10(5):108214. https://doi.org/10.1016/j.jece.2022.108214

  • Chekli L, Brunetti G, Marzouk ER, Maoz-Shen A, Smith E, Naidu R, Shon HK, Lombi E, Donner E (2016) Evaluating the mobility of polymer-stabilised zero-valent iron nanoparticles and their potential to co-transport contaminants in intact soil cores. Environ Pollut 216:636–645

    CAS  Google Scholar 

  • Davis JW (1993) Physico-chemical factors influencing ethylenediamine sorption to soil. Environ Toxicol Chem 12:27–35

    CAS  Google Scholar 

  • Dovi E, Aryee AA, Kani AN, Mpatani FM, Li J, Qu L, Han R (2022) High-capacity amino-functionalized walnut shell for efficient removal of toxic hexavalent chromium ions in batch and column mode. J Environ Chem Eng 10(2):107292. https://doi.org/10.1016/j.jece.2022.107292

  • Evans PE, Yost AJ, McElveen KA, Shi Q-Y, Ekanayaka TK, Manna AK, Schlegel V, Dowben PA, Lai RY, Varma S (2021) The role of amine in the sequestration of As (III) on functionalized indium tin oxide. Appl Surf Sci 538:147652. https://doi.org/10.1016/j.apsusc.2020.147652

  • Fajardo AR, Lopes LC, Pereira AGB, Rubira AF, Muniz EC (2012) Polyelectrolyte complexes based on pectin–NH2 and chondroitin sulfate. Carbohyd Polym 87:1950–1955

    CAS  Google Scholar 

  • Fang XB, Fang ZQ, Tsang PKE, Cheng W, Yan XM, Zheng LC (2014) Selective adsorption of Cr(VI) from aqueous solution by EDA-Fe3O4 nanoparticles prepared from steel pickling waste liquor. Appl Surf Sci 314:655–662

    CAS  Google Scholar 

  • Gil-Diaz M, Alonso J, Rodriguez-Valdes E, Gallego JR, Lobo MC (2017) Comparing different commercial zero valent iron nanoparticles to immobilize As and Hg in brownfield soil. Sci Total Environ 584–585:1324–1332

    Google Scholar 

  • Glaesner N, Donner E, Magid J, Rubaek GH, Zhang H, Lombi E (2012) Characterization of leached phosphorus from soil, manure, and manure-amended soil by physical and chemical fractionation and Diffusive Gradients in Thin films (DGT). Environ Sci Technol 46:10564–10571

    CAS  Google Scholar 

  • Gupta K, Joshi P, Gusain R, Khatri OP (2021) Recent advances in adsorptive removal of heavy metal and metalloid ions by metal oxide-based nanomaterials. Coord Chem Rev 445:214100. https://doi.org/10.1016/j.ccr.2021.214100

  • He Y, Gu F, Xu C, Chen J (2019) Influence of iron/aluminum oxides and aggregates on plant available water with different amendments in red soils. J Soil Water Conserv 74:145–159

    Google Scholar 

  • Ibrahim MM, El-Kemary MA, Al-Harbi SA, Al-Saidi HM, Sallam SA, Ramadan AE-MM (2021) Synthesis and structural characterization of pyridine-based Mn(III), Fe(III), and Co(III) complexes as SOD mimics and BSA binding studies. J Mol Struct 1228:129706. https://doi.org/10.1016/j.molstruc.2020.129706

  • Kocur CM, Chowdhury AI, Sakulchaicharoen N, Boparai HK, Weber KP, Sharma P, Krol MM, Austrins L, Peace C, Sleep BE, O’Carroll DM (2014) Characterization of nZVI mobility in a field scale test. Environ Sci Technol 48:2862–2869

    CAS  Google Scholar 

  • Kumpiene J, Carabante I, Kasiuliene A, Austruy A, Mench M (2021) Long-term stability of arsenic in iron amended contaminated soil. Environ Pollut 269:116017

    CAS  Google Scholar 

  • Li B, Zhou S, Wei D, Long J, Peng L, Tie B, Williams PN, Lei M (2019) Mitigating arsenic accumulation in rice (Oryza sativa L.) from typical arsenic contaminated paddy soil of southern China using nanostructured alpha-MnO2: Pot experiment and field application. Sci Total Environ 650:546–556

    CAS  Google Scholar 

  • Li Q, Liu H, Zhang L-C, Chen H, Zhu H, Wu Y, Xu M, Bao S-J (2020a) Highly efficient Fe-N-C oxygen reduction electrocatalyst engineered by sintering atmosphere. J Power Sour 449:227497

  • Li Q, Zhong H, Cao Y (2020b) Effects of the joint application of phosphate rock, ferric nitrate and plant ash on the immobility of As, Pb and Cd in soils. J Environ Manage 265:110576

    CAS  Google Scholar 

  • Li S, Lei X, Qin L, Sun X, Wang L, Zhao S, Wang M, Chen S (2021) Fe(III) reduction due to low pe+pH contributes to reducing Cd transfer within a soil-rice system. J Hazard Mater 415:125668

    CAS  Google Scholar 

  • Liang Q, Zhao D (2014) Immobilization of arsenate in a sandy loam soil using starch-stabilized magnetite nanoparticles. J Hazard Mater 271:16–23

    CAS  Google Scholar 

  • Liu M, Xu M, Zhang X, Zhou J, Ma Q, Wu L (2021) Poorly crystalline Fe() mineral phases induced by nano zero-valent iron are responsible for Cd stabilization with different soil moisture conditions and soil types. Ecotoxicol Environ Saf 223:112616

    CAS  Google Scholar 

  • Lobo C, Castellari J, Colman Lerner J, Bertola N, Zaritzky N (2020) Functional iron chitosan microspheres synthesized by ionotropic gelation for the removal of arsenic (V) from water. Int J Biol Macromol 164:1575–1583

    CAS  Google Scholar 

  • Mao S, Liu C, Wu Y, Xia M, Wang F (2022) Porous P, Fe-doped g-C3N4 nanostructure with enhanced photo-Fenton activity for removal of tetracycline hydrochloride: Mechanism insight DFT calculation and degradation pathways. Chemosphere 291:133039

    CAS  Google Scholar 

  • Masscheleyn PH, Delaune RD, Patrick WH (1991) Effect of redox potential and pH on arsenic speciation and solubility in a contaminated soil. Environ Sci Technol 25:1414–1419

    CAS  Google Scholar 

  • Nielsen SS, Petersen LR, Kjeldsen P, Jakobsen R (2011) Amendment of arsenic and chromium polluted soil from wood preservation by iron residues from water treatment. Chemosphere 84:383–389

    CAS  Google Scholar 

  • Otsuka R, Yoshitake H (2014) Different modes of adsorptions of arsenate on silica grafted with Fe3+-coordinated silanes. J Colloid Interface Sci 415:143–150

    CAS  Google Scholar 

  • Parambadath S, Mathew A, Kim SY, Park SS, Ha C-S (2018) Fe3+-bis-ethylenediamine complex bridged periodichromate. Pure Appl Chem 90:869–884

    CAS  Google Scholar 

  • Pfeifer H-R, Gueye-Girardet A, Reymond D, Schlegel C, Temgoua E, Hesterberg DL, Chou JW (2004) Dispersion of natural arsenic in the Malcantone watershed, Southern Switzerland: field evidence for repeated sorption–desorption and oxidation–reduction processes. Geoderma 122:205–234

    CAS  Google Scholar 

  • Rijith S, Anirudhan TS, Shripathi T (2012) Evaluation of iron(III) chelated polymer grafted lignocellulosics for arsenic(V) adsorption in a batch reactor system. Ind Eng Chem Res 51:10682–10694

    CAS  Google Scholar 

  • Safi SR, Senmoto K, Gotoh T, Iizawa T, Nakai S (2019) The effect of gamma-FeOOH on enhancing arsenic adsorption from groundwater with DMAPAAQ + FeOOH gel composite. Sci Rep 9:11909

    Google Scholar 

  • Seoudi R, El-Bahy GS, El Sayed ZA (2005) FTIR, TGA and DC electrical conductivity studies of phthalocyanine and its complexes. J Mol Struct 753:119–126

    CAS  Google Scholar 

  • Shan H, Liu Y, Zeng C, Peng S, Zhan H (2022) On As(III) adsorption characteristics of innovative magnetite graphene oxide chitosan microsphere. Materials (Basel) 15:7156

  • Shen B, Wang X, Zhang Y, Zhang M, Wang K, Xie P, Ji H (2020) The optimum pH and Eh for simultaneously minimizing bioavailable cadmium and arsenic contents in soils under the organic fertilizer application. Sci Total Environ 711:135229

    CAS  Google Scholar 

  • Somenahally AC, Hollister EB, Yan W, Gentry TJ, Loeppert RH (2011) Water management impacts on arsenic speciation and iron-reducing bacteria in contrasting rice-rhizosphere compartments. Environ Sci Technol 45:8328–8335

    CAS  Google Scholar 

  • TabatabaieeBafrooee AA, Moniri E, Ahmad Panahi H, Miralinaghi M, Hasani AH (2021) Ethylenediamine functionalized magnetic graphene oxide (Fe3O4@GO-EDA) as an efficient adsorbent in Arsenic(III) decontamination from aqueous solution. Res Chem Intermed 47:1397–1428

    CAS  Google Scholar 

  • Tabelin CB, Igarashi T, Takahashi R (2012) Mobilization and speciation of arsenic from hydrothermally altered rock in laboratory column experiments under ambient conditions. Appl Geochem 27:326–342

    CAS  Google Scholar 

  • Tang J, Zhang L, Zhang J, Ren L, Zhou Y, Zheng Y, Luo L, Yang Y, Huang H, Chen A (2020) Physicochemical features, metal availability and enzyme activity in heavy metal-polluted soil remediated by biochar and compost. Sci Total Environ 701:134751

    CAS  Google Scholar 

  • Tessier A, Campbell P, Bisson M (1979) Sequential extraction procedure for the speciation of particulate trace metals. Anal Chem 51:851

    Google Scholar 

  • Velázquez-Palenzuela A, Zhang L, Wang L, Cabot PL, Brillas E, Tsay K, Zhang J (2011) Carbon-supported Fe–Nx catalysts synthesized by pyrolysis of the Fe(II)–2,3,5,6-tetra(2-pyridyl)pyrazine complex: structure, electrochemical properties, and oxygen reduction reaction activity. J Phys Chem C 115:12929–12940

    Google Scholar 

  • Wang X, Liu Y, Zheng J (2016) Removal of As(III) and As(V) from water by chitosan and chitosan derivatives: a review. Environ Sci Pollut Res Int 23:13789–13801

    CAS  Google Scholar 

  • Wang Y, Liu Y, Su G, Yang K, Lin D (2021) Transformation and implication of nanoparticulate zero valent iron in soils. J Hazard Mater 412:125207

    CAS  Google Scholar 

  • Williams CD, Burton NA, Travis KP, Harding JH (2014) The development of a classical force field to determine the selectivity of an aqueous Fe(3+)-EDA complex for TcO4(-) and SO4(2.). J Chem Theory Comput 10:3345–3353

    CAS  Google Scholar 

  • Yamani JS, Lounsbury AW, Zimmerman JB (2016) Towards a selective adsorbent for arsenate and selenite in the presence of phosphate: assessment of adsorption efficiency, mechanism, and binary separation factors of the chitosan-copper complex. Water Res 88:889–896

    CAS  Google Scholar 

  • Yang D, Yang S, Yuan H, Wang F, Wang H, Xu J, Liu X (2021) Co-benefits of biochar-supported nanoscale zero-valent iron in simultaneously stabilizing soil heavy metals and reducing their bioaccessibility. J Hazard Mater 418:126292

    CAS  Google Scholar 

  • Yao BM, Wang SQ, Xie ST, Li G, Sun GX (2022) Optimal soil Eh, pH for simultaneous decrease of bioavailable Cd, As in co-contaminated paddy soil under water management strategies. Sci Total Environ 806:151342

    CAS  Google Scholar 

  • Zheng M, Huang Z, Ji H, Qiu F, Zhao D, Bredar ARC, Farnum BH (2020) Simultaneous control of soil erosion and arsenic leaching at disturbed land using polyacrylamide modified magnetite nanoparticles. Sci Total Environ 702:134997

    CAS  Google Scholar 

  • Zhou S, Du Y, Feng Y, Sun H, Xia W, Yuan H (2022) Stabilization of arsenic and antimony Co-contaminated soil with an iron-based stabilizer: assessment of strength, leaching and hydraulic properties and immobilization mechanisms. Chemosphere 301:134644

    CAS  Google Scholar 

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Funding

This study was supported by major projects of Ministry of Agriculture and Rural Affairs of the People’s Republic of China NK2022180401 and NK2022180404.

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The first draft of the manuscript was written by Qilin Lv. Tairan Zhou and Shuhan Wang contributed to the conception and design of the study. Material preparation, data collection, and analysis were performed by Yannig Ge and Tianhao Wang. Shuwen Hu and Xueqin Ren reviewed and edited the article. Yuping Song provided constructive suggestions. All authors read and approved the final manuscript.

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Correspondence to Shuwen Hu.

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Lv, Q., Zhou, T., Wang, T. et al. Immobilizing arsenic in soil via amine metal complex: a case study using iron-ethylenediamine. Environ Sci Pollut Res 30, 51942–51954 (2023). https://doi.org/10.1007/s11356-023-25986-7

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