نوع مقاله : مقاله پژوهشی

نویسندگان

1 گروه علوم خاک، دانشکده کشاورزی، دانشگاه فردوسی مشهد

2 استاد گروه علوم خاک، دانشکده کشاورزی، دانشگاه فردوسی مشهد

3 استادیار گروه علوم خاک دانشکده کشاورزی دانشگاه فردوسی مشهد

4 استاد گروه شیمی، دانشکده علوم، دانشگاه فردوسی مشهد

چکیده

مصرف بی­رویه کودهای آمونیومی، موجب ورود این نوع از آلاینده به اکوسیسیتم آبی و غنی شدن منابع آب می­گردد. در این پژوهش، جذب آمونیوم از محلول­های آبی بوسیله نانو ذرات اکسید آهن سنتز شده به روش شیمی سبز با استفاده از عصاره برگ اکالیپتوس گلوبلوس (EL-Fe NPs) ، به عنوان روشی جدید، سازگار با محیط زیست و مقرون به صرفه، بررسی شد. خصوصیات نانو ذرات توسط میکروسکوپ الکترونی عبوری (TEM)، طیف سنج پراش پرتو ایکس (XRD) و طیف سنج تبدیل فوریه مادون قرمز (FT-IR) تعیین شد. اثر زمان تماس (0- 120 دقیقه)، pH (3- 11) و نمک KCl به عنوان محلول زمینه بر جذب آمونیوم مورد بررسی قرار گرفت. داده­های حاصل از جذب آمونیوم توسط مدل­های سینتیکی برازش داده شدند. در شرایط pH تعادلی 7/3 جذب آمونیوم توسط EL-Fe NPs بعد از گذشت 30 دقیقه به تعادل رسید. در این مدت زمان، از غلظت اولیه 10 میلی­گرم بر لیتر آمونیوم، حدود 86/11% درصد آن توسط 5/1 گرم بر لیتر از نانو ذرات جذب شد. طبق نتایج، حذف آمونیوم تحت تاثیر pH و قدرت یونی (KCl) قرار داشت. به طوریکه در 8/7= pH حداکثر میزان جذب آلاینده (9/76 %) اتفاق افتاد. همچنین، افزایش قدرت یونی منجر به کاهش جذب آمونیوم گردید. به صورتی­که، در قدرت یونی­های 0، 001/0، 01/0 و 1/0 مولار KCl، میزان جذب به ترتیب 9/76، 2/64، 2/28 و 5 درصد بود. سینتیک جذب آمونیوم از معادله شبه مرتبه دوم تبعیت کرد (998/0 = r2). با توجه به اثر افزایش قدرت یونی در کاهش میزان جذب و همچنین وابسته بودن جذب آمونیوم به pH، انتظار می­رود که واکنش بین آمونیوم و EL-Feb NPs به احتمال زیاد از طریق الکترواستاتیک باشد. طبق نتایج، به­نظر می­رسد جذب آمونیوم توسط  EL-Fe NPs تحت تاثیر شیمی محلول قرار دارد.

کلیدواژه‌ها

موضوعات

عنوان مقاله [English]

Ammonium adsorption by green synthesized iron oxide nanoparticles with Eucalyptus globulus extracts from aqueous solutions

نویسندگان [English]

  • Ehsan Khoshkalam 1
  • amir fotovat 2
  • Akram Halajnia 3
  • Hossein Eshghi 4

1 Department of Soil Science, Faculty of Agriculture, Ferdowsi University of Mashhad

2 Professor, Department of Soil Science, Faculty of Agriculture, Ferdowsi University of Mashhad

3 Assistant Professor, Department of Soil Science, Agricultural College, Ferdowsi University of Mashhad

4 Professor, Department of Chemistry, Faculty of Science, Ferdowsi University of Mashhad

چکیده [English]

Improper use of ammonium fertilizer could cause this type of pollutant to enter the aquatic ecosystem and enriches water resources. In this research, ammonium adsorption by green synthesized iron oxide nanoparticles with Eucalyptus globulus (EL-Fe NPs) as innovative, inexpensive, and eco-friendly method, was investigated. Characterization of nanoparticles was determined by transmission electron microscopy (TEM), X-Ray diffraction (XRD), and Fourier-transform infrared spectroscopy (FT-IR). The effect of time (0-120), pH (3-11), and KCl salt as ionic strengths on ammonium adsorption by EL-Fe NPS was investigated. Also, kinetics models were fitted with ammonium adsorption data. The results showed iron oxide nanoparticles encapsulated by polyphenols from Eucalyptus globulus extract and have an irregular nanoparticulate structure with a size range between 50-100 nanometers. Ammonium adsorption by EL-Fe NPS was equilibrated at pH≈3.7 after 30 min and 11/86% ammonium was removed from 10 mg/L of initial concentration. Based on the results, this reaction is affected by pH and ionic strength (KCl). By increasing pH, Ammonium removal increased and at pH=7.8 maximum amount of pollutant (76.9%) was removed. Moreover, ionic strength had a contrary effect on ammonium adsorption. In the ionic strengths 0, 0.001, 0.01, and 0.1 ammonium adsorption 76.9, 64.2, 28.2, and 5% was decreased, respectively. These results depict ammonium and potassium compete for adsorption sites of EL-Fe NPs. The pseudo-second-order kinetic model provided a good description for ammonium adsorption (r2=0.998). Considering the effect of increasing the ionic strength in reducing the absorption rate and also the dependence of ammonium absorption on pH, it is expected that the reaction between ammonium and EL-Feb NPs is most likely through electrostatics. In general, it seems that Ammonium adsorption by EL-Fe NPs is influenced by solution chemistry.

کلیدواژه‌ها [English]

  • Ammonium adsorption
  • Eucalyptus globulus
  • Green synthesis
  • Iron oxide nanoparticles
  • Water pollution
Abida O., Van der Graaf F., and Li L.Y. 2020. Exploratory study of removing nutrients from aqueous environments employing a green synthesised nano zero-valent iron. Environmental Technology, 43(13): 2017-2032.
Ali I., and Gupta V.K. 2006. Advances in water treatment by adsorption technology. Nature protocols, 1(6): 2661-2667.
Arjaghi S.K., Alasl M.K., Sajjadi N., Fataei E., and Rajaei G.E. 2021. Green Synthesis of Iron Oxide Nanoparticles by RS Lichen Extract and its Application in Removing Heavy Metals of Lead and Cadmium. Biological Trace Element Research, 199(2): 763–768.
Bonilla-Petriciolet A., Mendoza-Castillo D.I., and Reynel-Ávila H.E. (Eds.). 2017. Adsorption processes for water treatment and purification (Vol. 256). Berlin: Springer.
Cao D., Jin X., Gan L., Wang T., and Chen Z. 2016. Chemosphere Removal of Phosphate Using Iron Oxide Nanoparticles Synthesized by Eucalyptus Leaf Extract in the Presence of CTAB Surfactant. Chemosphere, 159: 23–31.
Demirezen D.A., Yıldız Y.Ş., Yılmaz Ş., and Yılmaz D.D. 2019. Green Synthesis and Characterization of Iron Oxide Nanoparticles Using Ficus Carica (Common Fig) Dried Fruit Extract. Journal of Bioscience and Bioengineering, 127(2): 241–45.
Devatha C.P., Thalla A.K., and Katte S.Y. 2016. Green synthesis of iron nanoparticles using different leaf extracts for treatment of domestic waste water. Journal of Cleaner Production. 139: 1425-1435.
Dishon M., Zohar O., and Sivan U. 2009. From Repulsion to Attraction and Back to Repulsion: The Effect of NaCl, KCl, and CsCl on the Force between Silica Surfaces in Aqueous Solution. Langmuir, 25(5): 2831–2836.
Dong X., Ma L.Q., and Li Y. 2011. Characteristics and mechanisms of hexavalent chromium removal by biochar from sugar beet tailing. Journal of Hazardous Materials, 190(1–3): 909–915.
Ehrampoush M.H., Miria M., Salmani M.H., and Mahvi A.H. 2015. Cadmium Removal from Aqueous Solution by Green Synthesis Iron Oxide Nanoparticles with Tangerine Peel Extract. Journal of Environmental Health Science and Engineering, 13(1): 1–7.
Fahmy H.M., Mohamed F. M., Marzouq M.H., Mustafa A.B.E.D., Alsoudi A.M., Ali O.A., ... and Mahmoud F.A. 2018. Review of Green Methods of Iron Nanoparticles Synthesis and Applications. BioNanoScience, 8(2): 491–503.
Franco R.T., Silva A.L., Licea Y.E., Serna J.D.P., Alzamora M., Sánchez D.R., and Carvalho N.M.F. 2021. Green Synthesis of Iron Oxides and Phosphates via Thermal Treatment of Iron Polyphenols Synthesized by a Camellia sinensis Extract. Inorganic Chemistry, 60(8): 5734–5746.
Greenlee L.F., Lawler D.F., Freeman B.D., Marrot B., Moulin P., and Ce P. 2009. Reverse osmosis desalination : Water sources , technology , and today ’ s challenges. Water Research, 43(9): 2317–2348.
Guha T., Gopal G., Das H., Mukherjee A., and Kundu R. 2021. Nanopriming with zero-valent iron synthesized using pomegranate peel waste: A “green” approach for yield enhancement in Oryza sativa L. cv. Gonindobhog. Plant Physiology and Biochemistry, 163: 261–275.
Hoag G.E., Collins J.B., Holcomb J.L., Hoag J.R., Nadagouda M.N., and Varma R.S. 2009. Degradation of Bromothymol Blue by ‘greener’ Nano-Scale Zero-Valent Iron Synthesized Using Tea Polyphenols. Journal of Materials Chemistry, 19(45): 8671–8677.
Karpagavinayagam P., and Vedhi C. 2019. Green Synthesis of Iron Oxide Nanoparticles Using Avicennia Marina Flower Extract. Vacuum, 160: 286–292.
Jegadeesan G.B., Srimathi K., Santosh Srinivas N., Manishkanna S., and Vignesh D. 2019. Green synthesis of iron oxide nanoparticles using Terminalia bellirica and Moringa oleifera fruit and leaf extracts: Antioxidant, antibacterial and thermoacoustic properties. Biocatalysis and Agricultural Biotechnology, 21: 101-354
Khalil A., Sergeevich N., and Borisova V. 2018. Removal of ammonium from fish farms by biochar obtained from rice straw: Isotherm and kinetic studies for ammonium adsorption. Adsorption Science and Technology, 36(5–6): 1294–1309.
Khoshnam M., and Salimijazi H. 2021. Synthesis and characterization of magnetic-photocatalytic Fe3O4/SiO2/a-Fe2O3 nano core-shell. Surfaces and Interfaces, 26: 101-322.
Kononova O.N., Bryuzgina G.L., Apchitaeva O.V., and Kononov Y.S. 2019. Ion exchange recovery of chromium (VI) and manganese (II) from aqueous solutions. Arabian Journal of Chemistry, 12(8): 2713–2720.
Kulal P.M., Dubal D.P., Lokhande C.D., and Fulari V.J. 2011. Chemical synthesis of Fe2O3 thin films for supercapacitor application. Journal of Alloys and Compounds, 509(5): 2567–2571.
Luo F., Chen Z., Megharaj M., and Naidu R. 2016. Simultaneous removal of trichloroethylene and hexavalent chromium by green synthesized agarose-Fe nanoparticles hydrogel. Chemichal engineering journal, 294: 290–297.
Madhavi V., Prasad T.N.V.K.V., Reddy A.V.B., Reddy B.R., and Madhavi G. 2013. Application of Phytogenic Zerovalent Iron Nanoparticles in the Adsorption of Hexavalent Chromium. Spectrochimica Acta - Part A: Molecular and Biomolecular Spectroscopy, 116: 17–25.
Mahmoud A.E.D. 2020. Nanomaterials: Green Synthesis for Water Applications. Handbook of Nanomaterials and Nanocomposites for Energy and Environmental Applications. Springer International Publishing. pp. 1–21.
Manquián-Cerda K., Cruces E., Rubio M.A., Reyes C., and Arancibia-Miranda N. 2017. Preparation of Nanoscale Iron (Oxide, Oxyhydroxides and Zero-Valent) Particles Derived from Blueberries: Reactivity, Characterization and Removal Mechanism of Arsenate. Ecotoxicology and Environmental Safety, 145: 69–77.
Markova Z., Novak P., Kaslik J., Plachtova P., Brazdova M., Jancula D., Siskova K.M., Machala L., Marsalek B., Zboril R., and Varma R. 2014. Iron(II,III)-polyphenol complex nanoparticles derived from green tea with remarkable ecotoxicological impact. ACS Sustainable Chemistry and Engineering, 2(7): 1674–1680.
Martínez-Cabanas M., López-García M., Barriada J.L., Herrero R., and Sastre de Vicente M.E. 2016. Green synthesis of iron oxide nanoparticles. Development of magnetic hybrid materials for efficient As(V) removal. Chemical Engineering Journal, 301: 83–91.
Mondal P., Anweshan A., and Purkait M.K. 2020. Green synthesis and environmental application of iron-based nanomaterials and nanocomposite: a review. Chemosphere, 259: 127-509.
Mukherjee D., Ghosh S., Majumdar S., and Annapurna, K. 2016. Green synthesis of α-Fe2O3 nanoparticles for arsenic(V) remediation with a novel aspect for sludge management. Journal of Environmental Chemical Engineering, 4(1): 639–650.
Mystrioti C., Xanthopoulou T.D., Tsakiridis P.E., Papassiopi N., and Xenidis A. 2016. Comparative evaluation of five plant extracts and juices for nanoiron synthesis and application for hexavalent chromium reduction. Science of the Total Environment, 539: 105–113.
Nemeikaitė-Čėnienė A., Imbrasaitė A., Sergedienė E., and Čėnas N. 2005. Quantitative Structure-Activity Relationships in Prooxidant Cytotoxicity of Polyphenols: Role of Potential of Phenoxyl Radical/Phenol Redox Couple.” Archives of Biochemistry and Biophysics 441(2): 182–90.
Novak J.M., Busscher W.J., Watts D.W., Laird D.A., Ahmedna M.A., and Niandou M.A.S. 2010. Short-term CO2 mineralization after additions of biochar and switchgrass to a Typic Kandiudult. Geoderma, 154(3–4): 281–288.
Oncsik T., Trefalt G., Borkovec M., and Szilagyi I. 2015. Specific Ion Effects on Particle Aggregation Induced by Monovalent Salts within the Hofmeister Series. Langmuir, 31(13): 3799–3807.
Plachtová P., Medříková Z., Zbořil R., Tuček J., Varma R.S., and Maršálek B. 2018. Iron and Iron Oxide Nanoparticles Synthesized with Green Tea Extract: Differences in Ecotoxicological Profile and Ability to Degrade Malachite Green. ACS Sustainable Chemistry and Engineering, 6(7): 8679–8687.
Smernik R. 2003. Environmental Soil Chemistry. In Agriculture, Ecosystems and Environment (Vol. 100, Issue 1).
Verlag F., Britto D.T., and Kronzucker H.J. 2002. Review NH 4 + toxicity in higher plants : a critical review I . Introduction. 584(3): 44-57.
Vinayagam R., Zhou C., Pai S., Varadavenkatesan T., Narasimhan M.K., Narayanasamy S., and Selvaraj R. 2021. Structural characterization of green synthesized magnetic mesoporous Fe3O4NPs@ ME. Materials Chemistry and Physics, 262: 124-323.
Vocciante M., De Folly D’Auris A., Finocchi A., Tagliabue M., Bellettato M., Ferrucci A., Reverberi A.P., and Ferro S. 2018. Adsorption of ammonium on clinoptilolite in presence of competing cations: Investigation on groundwater remediation. Journal of Cleaner Production, 198: 480–487.
Walter W.G. 1961. Standards Methods for the Examination of Water and Wastewater (11th ed.). In American Journal of Public Health and the Nations Health (WEF, Vol. 51, Issue 6).
Wang H., Zhao X., Han X., Tang Z., Liu S., Guo W and Giesy J.P. 2017. Effects of Monovalent and Divalent Metal Cations on the Aggregation and Suspension of Fe3O4 Magnetic Nanoparticles in Aqueous Solution. Science of the Total Environment, 586: 817–26.
Wang L.K., Vaccari D.A., Li Y., and Shammas N.K. 2005. Chemical Precipitation. Physicochemical Treatment Processes, 3: 141–197.
Wang T., Jin X., Chen Z., Megharaj M., and Naidu R. 2014. Science of the Total Environment Green synthesis of Fe nanoparticles using eucalyptus leaf extracts for treatment of eutrophic wastewater. Science of the Total Environment, The, 466–467: 210–213.
Wang Z. 2013. Iron complex nanoparticles synthesized by eucalyptus leaves. ACS Sustainable Chemistry and Engineering, 1(12): 1551–1554.
Wang Z., Fang C., and Megharaj M. 2014. Characterization of iron-polyphenol nanoparticles synthesized by three plant extracts and their fenton oxidation of azo dye. ACS Sustainable Chemistry and Engineering, 2(4): 1022–1025.
Wang Z., Yu C., Fang C., and Mallavarapu M. 2014. Dye removal using iron-polyphenol complex nanoparticles synthesized by plant leaves. Environmental Technology and Innovation, 1–2(C): 29–34.
Whiteley C.G. and Lee D.J. 2006. Enzyme technology and biological remediation. Enzyme and Microbial Technology, 38(3-4): 291-316.
Xu Q., Li W., Ma L., Cao D., Owens G., and Chen Z. 2020. Simultaneous removal of ammonia and phosphate using green synthesized iron oxide nanoparticles dispersed onto zeolite. Science of the Total Environment, 703: 134-153.
Zhang R., Qi F., Liu C., Zhang Y., Wang Y., Song Z., and Kumirska J. 2019. Ecotoxicology and Environmental Safety Cyanobacteria derived taste anyd odor characteristics in various lakes in China : Songhua Lake , Chaohu Lake and Taihu Lake. Ecotoxicology and Environmental Safety, 181: 499–507.