Abstract
In this study, a ternary magnetically separable nanocomposite of silver nanoparticles (AgNPs) embedded in magnetic graphene oxide (Ag/Fe3O4@GO) was designed and synthesized. Beta-cyclodextrin was used as a green reducing and capping agent for decorating of AgNPs on Fe3O4@GO. The fabricated material was characterized using X-ray diffractometry, Fourier transform infrared spectroscopy, scanning electron microscopy, vibrating sample magnetometry, and energy-dispersive X-ray spectroscopy. The catalytic properties of the prepared Ag/Fe3O4@GO for the reduction of 4-nitrophenol (4-NP) and methylene blue (MB) dye with sodium borohydride were investigated in detail. The morphological and structural studies revealed that Fe3O4 and AgNPs with a mean size of 12 nm were uniformly distributed on the GO sheet at high densities. The catalytic tests showed that Ag/Fe3O4@GO exhibited an ultrafast catalytic reduction of 4-NP and MB with a reduction rate constant of 0.304 min−1 and 0.448 min−1, respectively. Moreover, the catalyst demonstrated excellent stability and reusability, as evidenced by the more than 97% removal efficiency maintained after five reuse cycles. The Ag/Fe3O4@GO catalyst could be easily recovered by the magnetic separation due to the superparamagnetic nature of Fe3O4 with high saturated magnetization (45.7 emu/g). Besides, the formation of networking between the formed AgNPs and β-CD through hydrogen bonding prevented the agglomeration of AgNPs, ensuring their high catalytic ability. The leaching study showed that the dissolution of Fe and Ag from Ag/Fe3O4@GO was negligible, indicating the environmental friendliness of the synthesized catalyst. Finally, the high catalytic performance, excellent stability, and recoverability of Ag/Fe3O4@GO make it a potential candidate for the reduction of organic pollutants in wastewater.
Similar content being viewed by others
Data Availability
All data generated or analyzed during this study are included in this published article.
References
Anh-Tran V, Vu KB, Vo TTT, Le VT, Do HH, Bach LG, Lee SW (2021) Experimental and computational investigation on interaction mechanism of Rhodamine B adsorption and photodegradation by zeolite imidazole frameworks-8. Appl Surf Sci 538:148065. https://doi.org/10.1016/j.apsusc.2020.148065
Cao M, Feng L, Yang P, Wang H, Liang X, Chen X (2018) Fabrication of reduced graphene oxide decorated with gold and nickel for the catalytic reduction of 4-nitrophenol. J Mater Sci 53:4874–4883. https://doi.org/10.1007/s10853-017-1913-9
Chengen HZL, Yun L, Leping H, Yingkui Y (2016) Graphene-supported silver nanoparticles with high activities toward chemical catalytic reduction of methylene blue and electrocatalytic oxidation of hydrazine. Int J Electrochem 11:9566–9574. https://doi.org/10.20964/2016.11.72
Choi Y, Bae HS, Seo E, Jang S, Park KH, Kim BS (2011) Hybrid gold nanoparticle-reduced graphene oxide nanosheets as active catalysts for highly efficient reduction of nitroarenes. J Mater Chem 21:15431–15436. https://doi.org/10.1039/C1JM12477C
Dao MU, Le HS, Hoang HY, Tran VA, Doan VD, Le TTN, Sirotkin A, Le VT (2020) Natural core-shell structure activated carbon beads derived from Litsea glutinosa seeds for removal of methylene blue: Facile preparation, characterization, and adsorption properties. Environ Res:110481. https://doi.org/10.1016/j.envres.2020.110481
Doan VD, Huynh BA, Nguyen TD, Cao XT, Nguyen VC, Nguyen TLH, Nguyen HT, Le VT (2020) Biosynthesis of silver and gold nanoparticles using aqueous extract of Codonopsis pilosula roots for antibacterial and catalytic applications. J Nanomater 2020:8492016–8492018. https://doi.org/10.1155/2020/8492016
Esmaeili N, Mohammadi P, Abbaszadeh M, Sheibani H (2019) Au nanoparticles decorated on magnetic nanocomposite (GO-Fe3O4/Dop/Au) as a recoverable catalyst for degradation of methylene blue and methyl orange in water. Int J Hydrog Energy 44:23002–23009. https://doi.org/10.1016/j.ijhydene.2019.07.025
Gan Z, Zhao A, Zhang M, Tao W, Guo H, Gao Q, Mao R, Liu E (2013) Controlled synthesis of Au-loaded Fe3O4@C composite microspheres with superior SERS detection and catalytic degradation abilities for organic dyes. Dalton Trans 42:8597–8605. https://doi.org/10.1039/C3DT50341K
Ismail M, Akhtar K, Khan MI, Kamal T, Khan MA, A MA, Seo J, Khan SB (2019) Pollution, toxicity and carcinogenicity of organic dyes and their catalytic bio-remediation. Curr Pharm Des 25:3645–3663. https://doi.org/10.2174/1381612825666191021142026
Kadam AN, Bhopate DP, Kondalkar VV, Majhi SM, Bathula CD, Tran AV, Lee SW (2018) Facile synthesis of Ag-ZnO core–shell nanostructures with enhanced photocatalytic activity. J Ind Eng Chem 61:78–86. https://doi.org/10.1016/j.jiec.2017.12.003
Kavyani S, Baharfar R (2020) Design and characterization of Fe3O4/GO/Au-Ag nanocomposite as an efficient catalyst for the green synthesis of spirooxindole-dihydropyridines. Appl Organomet Chem 34:e5560. https://doi.org/10.1002/aoc.5560
Kumari S, Sharma P, Yadav S, Kumar J, Vij A, Rawat P, Kumar S, Sinha C, Bhattacharya J, Srivastava CM, Majumder S (2020) A novel synthesis of the graphene oxide-silver (GO-Ag) nanocomposite for unique physiochemical applications. ACS Omega 5:5041–5047. https://doi.org/10.1021/acsomega.9b03976
Le TTN, Le VT, Dao MU, Nguyen QV, Vu TT, Nguyen MH, Tran DL, Le HS (2019) Preparation of magnetic graphene oxide/chitosan composite beads for effective removal of heavy metals and dyes from aqueous solutions. Chem Eng Commun 206:1337–1352. https://doi.org/10.1080/00986445.2018.1558215
Le VT, Doan VD, Tran VA, Le HS, Tran DL, Pham TM, Tran TH, Nguyen HT (2020) Cu/Fe3O4@carboxylate-rich carbon composite: one-pot synthesis, characterization, adsorption and photo-Fenton catalytic activities. Mater Res Bull 129:110913. https://doi.org/10.1016/j.materresbull.2020.110913
Lei G, Ma J, Li Z (2018) Magnetic Au-Ag-γ-Fe2O3/rGO Nanocomposites as an efficient catalyst for the Reduction of 4-Nitrophenol 8(11):877. https://doi.org/10.3390/nano8110877
Li N, Huang GW, Shen XJ, Xiao HM, Fu SY (2013) Controllable fabrication and magnetic-field assisted alignment of Fe3O4-coated Ag nanowires via a facile co-precipitation method. J Mater Chem C 1:4879–4884. https://doi.org/10.1039/C3TC30270A
Lim EB, Tran AV, Lee SW (2020) Comparative release kinetics of small drugs (ibuprofen and acetaminophen) from multifunctional mesoporous silica nanoparticles. J Mater Chem B 8:2096–2106. https://doi.org/10.1039/C9TB02494H
Liu G, Jiang W, Wang Y, Zhong S, Sun D, Liu J, Li F (2015) One-pot synthesis of Ag@Fe3O4/reduced graphene oxide composite with excellent electromagnetic absorption properties. Ceram Int 41:4982–4988. https://doi.org/10.1016/j.ceramint.2014.12.063
Liu YY, Zhao YH, Zhou Y, Guo XL, Chen ZT, Zhang WJ, Zhang Y, Chen J, Wang ZM, Sun LT, Zhang T (2018) High-efficient catalytic reduction of 4-nitrophenol based on reusable Ag nanoparticles/graphene-loading loofah sponge hybrid. Nanotechnology 29:315702. https://doi.org/10.1088/1361-6528/aac3e8
Luu TVH, Luu MD, Dao NN, Le VT, Nguyen HT, Doan VD (2020) Immobilization of C/Ce-codoped ZnO nanoparticles on multi-walled carbon nanotubes for enhancing their photocatalytic activity. J Dispers Sci Technol:1-12. https://doi.org/10.1080/01932691.2020.1740728
Ma YP, Mu BL, Zhang XJ, Xu HM, Qu Z, Gao L, Li B, Tian JJ (2019) Ag-Fe3O4@rGO ternary magnetic adsorbent for gaseous elemental mercury removal from coal-fired flue gas. Fuel 239:579–586. https://doi.org/10.1016/j.fuel.2018.11.065
Mao H, Ji C, Liu M, Cao Z, Sun D, Xing Z, Chen X, Zhang Y, Song X-M (2018) Enhanced catalytic activity of Ag nanoparticles supported on polyacrylamide/polypyrrole/graphene oxide nanosheets for the reduction of 4-nitrophenol. Appl Surf Sci 434:522–533. https://doi.org/10.1016/j.apsusc.2017.10.209
Nariya P, Das M, Shukla F, Thakore S (2020) Synthesis of magnetic silver cyclodextrin nanocomposite as catalyst for reduction of nitro aromatics and organic dyes. J Mol Liq 300:112279. https://doi.org/10.1016/j.molliq.2019.112279
Nguyen V-H, Thi Vo T-T, Huu Do H, Thuan Le V, Duy Nguyen T, Ky Vo T, Nguyen B-S, Tai Nguyen T, Khoa Phung T, Anh Tran V (2020) Ag@ZnO porous nanoparticle wrapped by rGO for the effective CO2 electrochemical reduction. Chem Eng Sci:116381. https://doi.org/10.1016/j.ces.2020.116381
Qu JC, Ren CL, Dong YL, Chang YP, Zhou M, Chen XG (2012) Facile synthesis of multifunctional graphene oxide/AgNPs-Fe3O4 nanocomposite: A highly integrated catalysts. Chem Eng J 211-212:412–420. https://doi.org/10.1016/j.cej.2012.09.096
Sharif HMA, Mahmood A, Cheng HY, Djellabi R, Ali J, Jiang WL, Wang SS, Haider MR, Mahmood N, Wang A-J (2019) Fe3O4 nanoparticles coated with EDTA and Ag nanoparticles for the catalytic reduction of organic dyes from wastewater. ACS Applied Nano Mater 2:5310–5319. https://doi.org/10.1021/acsanm.9b01250
Song S, Wang Y, Shen H, Zhang J, Mo H, Xie J, Zhou N, Shen J (2019) Ultrasmall graphene oxide modified with Fe3O4 nanoparticles as a fenton-like agent for methylene blue degradation. ACS Applied Nano Mater 2:7074–7084. https://doi.org/10.1021/acsanm.9b01608
Tran VA, Lee SW (2018) A prominent anchoring effect on the kinetic control of drug release from mesoporous silica nanoparticles (MSNs). J Colloid Interface Sci 510:345–356. https://doi.org/10.1016/j.jcis.2017.09.072
Tran AV, Shim K, Vo TTT, Kook JK, An SSA, Lee SW (2018) Targeted and controlled drug delivery by multifunctional mesoporous silica nanoparticles with internal fluorescent conjugates and external polydopamine and graphene oxide layers. Acta Biomater 74:397–413. https://doi.org/10.1016/j.actbio.2018.05.022
Tran VA, Kadam AN, Lee SW (2020a) Adsorption-assisted photocatalytic degradation of methyl orange dye by zeolite-imidazole-framework-derived nanoparticles. J Alloys Compd 835:155414. https://doi.org/10.1016/j.jallcom.2020.155414
Tran VA, Nguyen TP, Le VT, Kim I-T, Lee SW, Nguyen TC (2020b) Excellent photocatalytic activity of ternary Ag@WO3@rGO nanocomposites under solar simulation irradiation. J Sci Adv Mater Dev 6:108–117. https://doi.org/10.1016/j.jsamd.2020.12.001
Tran VA, Shim K, Lee SW, An SSA (2020c) Multimodal mesoporous silica nanocarriers for dual stimuli-responsive drug release and excellent photothermal ablation of cancer cells. Int J Nanomedicine 15:7667–7685. https://doi.org/10.2147/IJN.S254344
Tran VA, Tran NHT, Bach LG, Nguyen TD, Nguyen TT, Nguyen TT, Nguyen TAN, Vo TK, Vo TTT, Le VT (2020d) Facile synthesis of propranolol and novel derivatives. J Chem 2020:9597426–9597410. https://doi.org/10.1155/2020/9597426
Tran AV, Khoa PT, Thuan LV, Ky VT, Tai NT, Anh Nga NT, Quoc VD, Quang HV, Vo TTT (2021) Solar-light-driven photocatalytic degradation of methyl orange dye over Co3O4-ZnO nanoparticles. Mater Lett 284:128902. https://doi.org/10.1016/j.matlet.2020.128902
Veisi H, Razeghi S, Mohammadi P, Hemmati S (2019) Silver nanoparticles decorated on thiol-modified magnetite nanoparticles (Fe3O4/SiO2-Pr-S-Ag) as a recyclable nanocatalyst for degradation of organic dyes. Mater Sci Eng C 97:624–631. https://doi.org/10.1016/j.msec.2018.12.076
Xu S, Yong L, Wu P (2013) One-Pot, Green, Rapid synthesis of flowerlike gold nanoparticles/reduced graphene oxide composite with regenerated silk fibroin as efficient oxygen reduction electrocatalysts. ACS Appl Mater Interfaces 5:654–662. https://doi.org/10.1021/am302076x
Xu Y, Shi X, Hua R, Zhang R, Yao Y, Zhao B, Liu T, Zheng J, Lu G (2020) Remarkably catalytic activity in reduction of 4-nitrophenol and methylene blue by Fe3O4@COF supported noble metal nanoparticles. Appl Catal B Environ 260:118142. https://doi.org/10.1016/j.apcatb.2019.118142
Yazdani F, Seddigh M (2016) Magnetite nanoparticles synthesized by co-precipitation method: The effects of various iron anions on specifications. Mater Chem Phys 184:318–323. https://doi.org/10.1016/j.matchemphys.2016.09.058
Zhu M, Wang C, Meng D, Diao G (2013) In situ synthesis of silver nanostructures on magnetic Fe3O4@C core–shell nanocomposites and their application in catalytic reduction reactions. J Mater Chem A 1:2118–2125. https://doi.org/10.1039/C2TA00669C
Funding
This research is funded by Vietnam National Foundation for Science and Technology Development (NAFOSTED) under grant number 104.05-2019.03.
Author information
Authors and Affiliations
Contributions
All authors contributed to the study conception and design. Material preparation, data collection, and analysis were performed by Van Dat Doan, Ngoc Vy Nguyen, and Thi Lan Huong Nguyen. The first draft of the manuscript was written by Van Thuan Le, and all authors commented on previous versions of the manuscript. Writing—review and editing was performed by Vy Anh Tran. All authors read and approved the final manuscript.
Corresponding authors
Ethics declarations
Ethics approval and consent to participate
Not applicable
Consent for publication
Not applicable
Competing interests
The authors declare no competing interests.
Additional information
Responsible Editor: Santiago V. Luis
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Doan, VD., Nguyen, NV., Nguyen, T.LH. et al. High-efficient reduction of methylene blue and 4-nitrophenol by silver nanoparticles embedded in magnetic graphene oxide. Environ Sci Pollut Res 30, 71543–71553 (2023). https://doi.org/10.1007/s11356-021-13597-z
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-021-13597-z