Abstract
Dyeing wastewaters present high hazards for the environment and human health. Advanced dye removal may be achieved by magnetic metal–organic frameworks (MMOFs) due to their high adsorption and catalyst efficiencies. However, the existing synthesis strategies of frameworks are often cumbersome and time-consuming in the presence of toxic solvents. Hence, a simple and environmentally-friendly synthetic method is desired. Here, a kind of MMOF, Fe3O4/Cu3(BTC)2 (BTC = 1,3,5-benzenetricarboxylate), was synthesized via a novel aqueous solution-phase synthesis. The product Fe3O4/Cu3(BTC)2 has a high specific surface area of 755.15 m2 g−1, and excellent magnetic performance of 31.2 emu g−1. The Fe3O4/Cu3(BTC)2 can effectively remove methylene blue from wastewater in the presence of H2O2. After having been finished the dye removal, it was easily separated and recycled several times by use of the magnetic technology.
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11 December 2018
In the Acknowledgements section in the original article, the Grant number Y19E030048 is incorrect.
References
Cao X, Tan C, Sindoro M, Zhang H (2018) Correction: hybrid micro-/nano-structures derived from metal–organic frameworks: preparation and applications in energy storage and conversion. Chem Soc Rev 46(10):2660. https://doi.org/10.1039/C6CS00426A
Chen Y, Huang X, Feng X, Li J, Huang Y, Zhao J, Guo Y, Dong X, Han R, Qi P (2014) Facile fabrication of magnetically recyclable metal–organic framework nanocomposites for highly efficient and selective catalytic oxidation of benzylic C–H bonds. Chem Commun 50(61):8374–8377. https://doi.org/10.1039/c4cc03728f
Cheng M, Lai C, Liu Y, Zeng G, Huang D, Zhang C, Qin L, Hu L, Zhou C, Xiong W (2018) Metal-organic frameworks for highly efficient heterogeneous Fenton-like catalysis. Coord Chem Rev 368:80–92. https://doi.org/10.1016/j.ccr.2018.04.012
Chui SS-Y, Lo SM-F, Charmant JP, Orpen AG, Williams ID (1999) A chemically functionalizable nanoporous material [Cu3(TMA)2(H2O)3]n. Science 283(5405):1148–1150. https://doi.org/10.1126/science.283.5405.1148
Cui K, Yan B, Xie Y, Qian H, Wang X, Huang Q, He Y, Jin S, Zeng H (2018) Regenerable urchin-like Fe3O4@ PDA-Ag hollow microspheres as catalyst and adsorbent for enhanced removal of organic dyes. J Hazard Mater. https://doi.org/10.1016/j.jhazmat.2018.02.011
Feng M, Zhang P, Zhou HC, Sharma VK (2018) Water-stable metal-organic frameworks for aqueous removal of heavy metals and radionuclides: a review. Chemosphere 209:783. https://doi.org/10.1016/j.chemosphere.2018.06.114
Jiang Z, Li Y (2016) Facile synthesis of magnetic hybrid Fe3O4/MIL-101 via heterogeneous coprecipitation assembly for efficient adsorption of anionic dyes. J Taiwan Inst Chem Eng 59:373–379. https://doi.org/10.1016/j.jtice.2015.09.002
Jiang X, Chen H-Y, Liu L-L, Qiu L-G, Jiang X (2015) Fe3O4 embedded ZIF-8 nanocrystals with ultra-high adsorption capacity towards hydroquinone. J Alloys Compd 646:1075–1082. https://doi.org/10.1016/j.jallcom.2015.06.021
Jiangbo H, Haojie C, Minglai F, Baoling Y (2017) The fabrication of magnetic metal-organic frameworks composites and their application in environment. Sci Sin Chim 47(7):830–843. https://doi.org/10.1360/N032016-00199
Ke F, Qiu L-G, Yuan Y-P, Jiang X, Zhu J-F (2012) Fe3O4@ MOF core–shell magnetic microspheres with a designable metal–organic framework shell. J Mater Chem 22(19):9497–9500. https://doi.org/10.1039/C2JM31167D
Li L, Liu XL, Geng HY, Hu B, Song GW, Xu ZS (2013) A MOF/graphite oxide hybrid (MOF: HKUST-1) material for the adsorption of methylene blue from aqueous solution. J Mater Chem A 1(35):10292–10299. https://doi.org/10.1039/C3TA11478C
Liu X, Zhou Y, Zhang J, Lin T, Lin L, Zeng G (2017) Iron containing metal-organic frameworks: structure, synthesis, and applications in environmental remediation. ACS Appl Mater Interfaces. https://doi.org/10.1021/acsami.7b02563
Majano G, Pérez-Ramírez J (2013) Scalable room-temperature conversion of copper (II) hydroxide into HKUST-1 (Cu3(btc)2). Adv Mater 25(7):1052–1057. https://doi.org/10.1002/adma.201203664
Maurin G, Serre C, Cooper A, Férey G (2017) The new age of MOFs and of their porous-related solids. Chem Soc Rev 46(11):3104–3107. https://doi.org/10.1039/C7CS90049J
Okada K, Ricco R, Tokudome Y, Styles MJ, Hill AJ, Takahashi M, Falcaro P (2014) Copper conversion into Cu(OH)2 nanotubes for positioning Cu3(BTC)2 MOF crystals: controlling the growth on flat plates, 3D architectures, and as patterns. Adv Funct Mater 24(14):1969–1977. https://doi.org/10.1002/adfm.201303303
Pang F, He M, Ge J (2015) Controlled synthesis of Fe3O4/ZIF-8 nanoparticles for magnetically separable nanocatalysts. Chem Eur J 21(18):6879–6887. https://doi.org/10.1002/chem.201405921
Sham AYW, Notley SM (2018) Adsorption of organic dyes from aqueous solutions using surfactant exfoliated graphene. J Environ Chem Eng 6(1):495–504. https://doi.org/10.1016/j.jece.2017.12.028
Shao Y, Zhou L, Bao C, Ma J, Liu M, Wang F (2016) Magnetic responsive metal-organic frameworks nanosphere with core-shell structure for highly efficient removal of methylene blue. Chem Eng J 283:1127–1136. https://doi.org/10.1016/j.cej.2015.08.051
Wang L, Bao J, Wang L, Zhang F, Li Y (2006) One-pot synthesis and bioapplication of amine-functionalized magnetite nanoparticles and hollow nanospheres. Chem Eur J 12(24):6341–6347. https://doi.org/10.1002/chem.200501334
Wu G, Ma J, Li S, Guan J, Jiang B, Wang L, Li J, Wang X, Chen L (2018) Magnetic copper-based metal organic framework as an effective and recyclable adsorbent for removal of two fluoroquinolone antibiotics from aqueous solutions. J Colloid Interface Sci. https://doi.org/10.1016/j.jcis.2018.05.105
Yang Q, Zhao Q, Ren S, Lu Q, Guo X, Chen Z (2016) Fabrication of core-shell Fe3O4@ MIL-100 (Fe) magnetic microspheres for the removal of Cr(VI) in aqueous solution. J Solid State Chem 244:25–30. https://doi.org/10.1016/j.jssc.2016.09.010
Yang Q, Wang Y, Wang J, Liu F, Hu N, Pei H, Yang W, Li Z, Suo Y, Wang J (2018) High effective adsorption/removal of illegal food dyes from contaminated aqueous solution by Zr-MOFs (UiO-67). Food Chem 254:241–248. https://doi.org/10.1016/j.foodchem.2018.02.011
Zhang T, Lin L, Zhang X, Liu H, Yan X, Qiu J, Yeung KL (2015a) Synthesis and characterization of ZIF-8@ SiO2@ Fe3O4core @ double-shell microspheres with noble metal nanoparticles sandwiched between two shell layers. Mater Lett 148:17–21. https://doi.org/10.1016/j.matlet.2015.02.077
Zhang W, Yan Z, Gao J, Tong P, Liu W, Zhang L (2015b) Metal-organic framework UiO-66 modified magnetite@ silica core-shell magnetic microspheres for magnetic solid-phase extraction of domoic acid from shellfish samples. J Chromatogr A 1400:10–18. https://doi.org/10.1016/j.chroma.2015.04.061
Acknowledgements
This work was financially supported by the Zhejiang province public welfare technology application research project (Grant Numbers. 2017C33077) and Zhejiang Provincial Natural Science Foundation of China (Grant Numbers. Y19E030048). We would like to thank Hasan Md Mehedi for his suggestion on the writing and grammar of the article.
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Sun, H., Zhang, H., Mao, H. et al. Facile synthesis of the magnetic metal–organic framework Fe3O4/Cu3(BTC)2 for efficient dye removal. Environ Chem Lett 17, 1091–1096 (2019). https://doi.org/10.1007/s10311-018-00833-1
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DOI: https://doi.org/10.1007/s10311-018-00833-1