Magnetic KIT-6 nano-composite and its amino derivatives as convenient adsorbent for U(VI) sequestration

Abstract

Although mesoporous silica with magnetically hybridized two-dimensional channel structures has been well studied in recent years, it remains a challenge to fabricate the counterpart with macroporous three-dimensional cubic structures since the highly acidic preparation conditions lead to dissolution of magnetic particles. Herein, we successfully prepared magnetic KIT-6 nano-composite and its amino derivatives by bearing acid-resistant iron oxide. The prepared materials exhibited excellent properties for U(VI) ions removal from aqueous solutions under various conditions. The experimental data show that the U(VI) adsorption features fast adsorption kinetics, high adsorption capacity and ideal selectivity toward U(VI). The adsorption process is of spontaneous and endothermic nature and ionic strength independence, and the adsorbents can be easily regenerated by acid treatment. Compared to pristine KIT-6, the introduction of magnetism does not reduce the efficiency of the material to remove U(VI) while exerting its role as a recovery adsorbent. The findings of this work further demonstrate the potential broad application prospects of magnetic hybrid mesoporous silica in radionuclide chelation.

Graphical abstract

Keywords

magnetic nanoparticle / 3D mesoporous silica / amino functionalization / adsorption of U(VI) / acid resistance

References

[1] Dilshani A, Wijayananda A, Rathnayake M. Life cycle net energy and global warming impact assessment for hydrogen production via decomposition of ammonia recovered from source-separated human urine. International Journal of Hydrogen Energy, 2022, 47(57): 24093–24106

[2] Zhao B, Yuan L Y, Wang Y, Duan T, Shi W Q. Carboxylated UiO-66 tailored for U(VI) and Eu(III) trapping: from batch adsorption to dynamic column separation. ACS Applied Materials & Interfaces, 2021, 13(14): 16300–16308

[3] Mei P, Xiao J T, Huang X S, Ishag A, Sun Y B. Enhanced photocatalytic reduction of U(VI) on SrTiO₃/g-C₃N₄ composites: synergistic interaction. European Journal of Inorganic Chemistry, 2022, 2022(7): e202101005

[4] Chandrasekar A, Suresh A, Joshi M, Sundararajan M, Ghanty T K, Sivaraman N. Highly selective separations of U(VI) from a Th(IV) matrix by branched butyl phosphates: insights from solvent extraction, chromatography and quantum chemical calculations. Separation and Purification Technology, 2019, 210: 182–194

[5] Sharma N, Ghosh A, Fortner J D, Giammar D E. Modeling performance of rhamnolipid-coated engineered magnetite nanoparticles for U(VI) sorption and separation. Environmental Science. Nano, 2020, 7(7): 2010–2020

[6] Gomes Rodrigues D, Monge S, Dacheux N, Pellet-Rostaing S, Faur C. Highlighting the selective properties of carbamoylmethylphosphonated hydrosoluble polymers for Gd(III)/Th(IV)/U(VI) separation. Separation and Purification Technology, 2021, 254: 117260

[7] Guo Y D, Li S H, Yang F, Li C X, Guo Y P, Xuan K, Wang G H, Liu Y H, Li J. Efficient charge separation in sulfur doped AgFeO₂ photocatalyst for enhanced photocatalytic U(VI) reduction: the role of doping and mechanism insights. Journal of Hazardous Materials, 2022, 440: 129734

[8] Su M H, Li H, Liu Z Q, Peng H R, Huang S, Zhou Y, Liao C Z, Song G, Chen D Y. Highly-efficient and easy separation of gamma-Fe₂O₃ selectively adsorbs U(VI) in waters. Environmental Research, 2022, 210: 112917

[9] Chen G, Weng H Q, Wu Z H, Chen Y Z, Zhang P, Ye G A, Lin M Z. High-yield production of monolayer boron nitride nanosheets by cationic-surfactant-assisted solvothermal exfoliation for the ultrafast and selective separation of U(VI) from lanthanides. Separation and Purification Technology, 2022, 278: 119645

[10] Guo L J, Peng L Q, Li J H, Zhang W H, Shi B. Simultaneously efficient adsorption and highly selective separation of U(VI) and Th(IV) by surface-functionalized lignin nanoparticles: a novel pH-dependent process. Journal of Hazardous Materials, 2023, 443: 130123

[11] Chen Z S, Wang J Y, Hao M J, Xie Y H, Liu X L, Yang H, Waterhouse G I N, Wang X K, Ma S Q. Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance. Nature Communications, 2023, 14(1): 1106

[12] Yang H, Hao M J, Xie Y H, Liu X L, Liu Y F, Chen Z S, Wang X K, Waterhouse G I N, Ma S Q. Tuning local charge distribution in multicomponent covalent organic frameworks for dramatically enhanced photocatalytic uranium extraction. Angewandte Chemie-International Edition, 2023, 62(30): e202303129

[13] Li W, Zhao D Y. An overview of the synthesis of ordered mesoporous materials. Chemical Communications, 2013, 49(10): 943–946

[14] Hoffmann F, Cornelius M, Morell J, Froba M. Silica-based mesoporous organic-inorganic hybrid materials. Angewandte Chemie International Edition, 2006, 45(20): 3216–3251

[15] Makowski P, Deschanels X, Grandjean A, Meyer D, Toquer G, Goettmann F. Mesoporous materials in the field of nuclear industry: applications and perspectives. New Journal of Chemistry, 2012, 36(3): 531–541

[16] Koike N, Ikuno T, Okubo T, Shimojima A. Synthesis of monodisperse organosilica nanoparticles with hollow interiors and porous shells using silica nanospheres as templates. Chemical Communications, 2013, 49(44): 4998–5000

[17] Liu Y L, Yuan L Y, Yuan Y L, Lan J H, Li Z J, Feng Y X, Zhao Y L, Chai Z F, Shi W Q. A high efficient sorption of U(VI) from aqueous solution using amino-functionalized SBA-15. Journal of Radioanalytical and Nuclear Chemistry, 2012, 292(2): 803–810

[18] Lebed P J, De Souza K, Bilodeau F, Lariviere D, Kleitz F. Phosphonate-functionalized large pore 3-D cubic mesoporous (KIT-6) hybrid as highly efficient actinide extracting agent. Chemical Communications, 2011, 47(41): 11525–11527

[19] Yang X, Su J, Xiong J J, Wang H B. Preparation of nano-silica with radial wrinkle structures for self-cleaning and superhydrophobic coatings. Fibers and Polymers, 2022, 23(5): 1293–1299

[20] Yuan L Y, Liu Y L, Shi W Q, Lv Y L, Lan J H, Zhao Y L, Chai Z F. High performance of phosphonate-functionalized mesoporous silica for U(VI) sorption from aqueous solution. Dalton Transactions, 2011, 40(28): 7446–7453

[21] Yuan L Y, Zhu L, Xiao C L, Wu Q Y, Zhang N, Yu J P, Chai Z F, Shi W Q. Large-pore 3D cubic mesoporous (KIT-6) hybrid bearing a hard-soft donor combined ligand for enhancing U(VI) capture: an experimental and theoretical investigation. ACS Applied Materials & Interfaces, 2017, 9(4): 3774–3784

[22] Hegde V, Pandit P, Rananaware P, Brahmkhatri V P. Sulfonic acid-functionalized mesoporous silica catalyst with different morphology for biodiesel production. Frontiers of Chemical Science and Engineering, 2022, 16(8): 1198–1210

[23] Yuan L Y, Liu Y L, Shi W Q, Li Z J, Lan J H, Feng Y X, Zhao Y L, Yuan Y L, Chai Z F. A novel mesoporous material for uranium extraction, dihydroimidazole functionalized SBA-15. Journal of Materials Chemistry, 2012, 22(33): 17019–17026

[24] Wang X L, Yuan L Y, Wang Y F, Li Z J, Lan J H, Liu Y L, Feng Y X, Zhao Y L, Chai Z F, Shi W Q. Mesoporous silica SBA-15 functionalized with phosphonate and amino groups for uranium uptake. Science China. Chemistry, 2012, 55(9): 1705–1711

[25] Zhang W, Ye G, Chen J. Novel mesoporous silicas bearing phosphine oxide ligands with different alkyl chains for the binding of uranium in strong HNO₃ media. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 2013, 1(41): 12706–12709

[26] Vivero-Escoto J L, Carboni M, Abney C W, Dekrafft K E, Lin W B. Organo-functionalized mesoporous silicas for efficient uranium extraction. Microporous and Mesoporous Materials, 2013, 180: 22–31

[27] Chen S W, Guo B L, Wang Y L, Li Y, Song L J. Study on sorption of U(VI) onto ordered mesoporous silicas. Journal of Radioanalytical and Nuclear Chemistry, 2013, 295(2): 1435–1442

[28] Lebed P J, Savoie J D, Florek J, Bilodeau F, Lariviere D, Kleitz F. Large pore mesostructured organosilica-phosphonate hybrids as highly efficient and regenerable sorbents for uranium sequestration. Chemistry of Materials, 2012, 24(21): 4166–4176

[29] Cui J S, Li W K, Song X L, Zhang Z T, Yu H B, Shan W J, Xiong Y. Microwave-assisted one-pot rapid synthesis of mesoporous silica-chitosan composites for efficient recovery of rhenium(VII). Separation and Purification Technology, 2021, 277: 119497

[30] Xiong Y, Xie L S, Zhu L, Wang Y J, Shan W J, Lou Z N, Cui J S, Yu H B. Superior adsorption of Re(VII) by anionic imprinted chitosan-silica composite: adsorption performance, selectivity and mechanism study. Journal of Industrial and Engineering Chemistry, 2022, 108: 344–355

[31] Showkat A M, Zhang Y P, Kim M S, Gopalan A I, Reddy K R, Lee K P. Analysis of heavy metal toxic ions by adsorption onto amino-functionalized ordered mesoporous silica. Bulletin of the Korean Chemical Society, 2007, 28(11): 1985–1992

[32] Kothalawala N, Blitz J P, Gun’ko V M, Jaroniec M, Grabicka B, Semeniuc R F. Post-synthesis surface-modified silicas as adsorbents for heavy metal ion contaminants Cd(II), Cu(II), Cr(III), and Sr(II) in aqueous solutions. Journal of Colloid and Interface Science, 2013, 392: 57–64

[33] Bae J A, Song K C, Jeon J K, Ko Y S, Park Y K, Yim J H. Effect of pore structure of amine-functionalized mesoporous silica-supported rhodium catalysts on 1-octene hydroformylation. Microporous and Mesoporous Materials, 2009, 123(1–3): 289–297

[34] Kitt J P, Harris J M. Confocal raman microscopy for in situ detection of solid-phase extraction of pyrene into single C-18-silica particles. Analytical Chemistry, 2014, 86(3): 1719–1725

[35] Zhang P C, Wang L, Du K, Wang S Y, Huang Z W, Yuan L Y, Li Z J, Wang H Q, Zheng L R, Chai Z F, Shi W. Effective removal of U(VI) and Eu(III) by carboxyl functionalized MXene nanosheets. Journal of Hazardous Materials, 2020, 396: 122731

[36] Kim D I, Park J H, Kim S D, Lee J Y, Yim J H, Jeon J K, Park S H, Park Y K. Comparison of removal ability of indoor formaldehyde over different materials functionalized with various amine groups. Journal of Industrial and Engineering Chemistry, 2011, 17(1): 1–5

[37] Zhao Y, Zhai S R, Zhai B, An Q D. Heavy metal removal of tri-amino-functionalized sol-gel hybrids with tailored characteristics. Journal of Sol-Gel Science and Technology, 2012, 62(2): 177–185

[38] Sun Y, Liu X, Sun C G, Al-Sarraf W, Foo K Z, Meng Y, Lee S, Wang W L, Liu H. Synthesis and functionalisation of spherical meso-, hybrid meso/macro- and macro-porous cellular silica foam materials with regulated pore sizes for CO₂ capture. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 2018, 6(46): 23587–23601

[39] Wang G, Otuonye A N, Blair E A, Denton K, Tao Z M, Asefa T. Functionalized mesoporous materials for adsorption and release of different drug molecules: a comparative study. Journal of Solid State Chemistry, 2009, 182(7): 1649–1660

[40] Leal O, Bolivar C, Ovalles C, Garcia J J, Espidel Y. Reversible adsorption of carbon dioxide on amine surface-bonded silica gel. Inorganica Chimica Acta, 1995, 240(1–2): 183–189

[41] Popa A, Borcanescu S, Holclajtner-Antunovic I, Bajuk-Bogdanovic D, Uskokovic-Markovic S. Preparation and characterisation of amino-functionalized pore-expanded mesoporous silica for carbon dioxide capture. Journal of Porous Materials, 2021, 28(1): 143–156

[42] Huang Y F, Zhang B, Liu B B, Han G H, Du Y F, Su S P. Adsorption behaviors of strategic W/Mo/Re from wastewaters by novel magnetic ferrite nanoparticles: adsorption mechanism underlying selective separation. Journal of Hazardous Materials, 2022, 424: 127675

[43] Nekounam H, Babaei M, Kisomi M F, Pourkhodadad S, Mahmoodi N, Nazbar A, Hasanzadeh E, Zarei M, Faridi-Majidi R. Application of functional magnetic nanoparticles for separation of target materials: a review. Current Nanoscience, 2022, 18(5): 554–570

[44] Liu T T, Liu L H, Liu J, Liu S M, Qiao S Z. Fe₃O₄ encapsulated mesoporous silica nanospheres with tunable size and large void pore. Frontiers of Chemical Science and Engineering, 2014, 8(1): 114–122

[45] Liang S, Ziyu Z, Han J, Xiaoyan D. Facile synthesis of magnetic mesoporous silica spheres for efficient removal of methylene blue via catalytic persulfate activation. Separation and Purification Technology, 2021, 256: 117801

[46] Radoń A, Łoński S, Kądziołka-Gaweł M, Gębara P, Lis M, Łukowiec D, Babilas R. Influence of magnetite nanoparticles surface dissolution, stabilization and functionalization by malonic acid on the catalytic activity, magnetic and electrical properties. Colloids and Surfaces. A, Physicochemical and Engineering Aspects, 2020, 607: 125446

[47] Ji G J, Zhu G R, Wang X H, Wei Y L, Yuan J S, Gao C J. Preparation of amidoxime functionalized SBA-15 with platelet shape and adsorption property of U(VI). Separation and Purification Technology, 2017, 174: 455–465

[48] Li D E, Egodawatte S, Kaplan D I, Larsen S C, Serkiz S M, Seaman J C, Scheckel K G, Lin J R, Pan Y M. Sequestration of U(VI) from acidic, alkaline, and high ionic-strength aqueous media by functionalized magnetic mesoporous silica nanoparticles: capacity and binding mechanisms. Environmental Science & Technology, 2017, 51(24): 14330–14341

[49] Liu F L, Wang A J, Xiang M, Hu Q Y, Hu B W. Effective adsorption and immobilization of Cr(VI) and U(VI) from aqueous solution by magnetic amine-functionalized SBA-15. Separation and Purification Technology, 2022, 282: 120042

[50] Zhao Y G, Li J X, Zhang S W, Wang X K. Amidoxime-functionalized magnetic mesoporous silica for selective sorption of U(VI). RSC Advances, 2014, 4(62): 32710–32717

[51] Zhou L M, Ouyang J B, Liu Z R, Huang G L, Wang Y, Li Z, Adesina A A. Highly efficient sorption of U(VI) from aqueous solution using amino/amine-functionalized magnetic mesoporous silica nanospheres. Journal of Radioanalytical and Nuclear Chemistry, 2019, 319(3): 987–995

[52] Sugimoto T, Matijevic E. Formation of uniform spherical magnetite particles by crystallization from ferrous hydroxide gels. Journal of Colloid and Interface Science, 1980, 74(1): 227–243

[53] Guo W L, Nie C M, Wang L, Li Z J, Zhu L, Zhu L Z, Zhu Z T, Shi W Q, Yuan L Y. Easily prepared and stable functionalized magnetic ordered mesoporous silica for efficient uranium extraction. Science China. Chemistry, 2016, 59(5): 629–636

Competing interests

The authors declare that they have no competing interests.

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant Nos. 22276193, U20B2019, and U2067212) and the National Science Fund for Distinguished Young Scholars (Grant No. 21925603).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at http://doi.org/10.1007/s11705-023-2358-0 and accessible for authorized users.

RIGHTS & PERMISSIONS

2023 Higher Education Press