Abstract
In this work, solar light induced photoreduction of water-soluble U(VI) was realized with metahnol under anaerobic conditions at the optimal pH around 5.00. TEM, XPS, and XRD analyses prove that U(VI) is removed from the aqueous solution by forming insoluble brown uranium precipitates containing uranium dioxide (UO2). The photoreduction approach shows obvious selectivity for the removal of U(VI) and the efficiency (95.47%) is comparable to that of the photocatalytic reduction method (99.35%) while only uranium sediments are formed with the photoreduction approach. Photoreduction offers an efficient approach for the rapid removal of U(VI) from the aqueous solution.
Similar content being viewed by others
References
Tollefson J (2016) China’s carbon emissions could peak sooner than forecast. Nature 531(7595):425–425
Butler D (2004) Nuclear power’s new dawn. Nature 429(6989):238–240
Li Z-J, Huang Z-W, Guo W-L, Wang L, Zheng L-R, Chai Z-F, Shi W-Q (2017) Enhanced photocatalytic removal of uranium(VI) from aqueous solution by magnetic TiO2/Fe3O4 and its graphene composite. Environ Sci Technol 51(10):5666–5674
Dewey C, Sokaras D, Kroll T, Bargar JR, Fendorf S (2020) Calcium-uranyl-carbonato species kinetically limit U(VI) reduction by Fe(II) and lead to U(V)-bearing ferrihydrite. Environ Sci Technol 54(10):6021–6030
O’Loughlin EJ, Kelly SD, Cook RE, Csencsits R, Kemner KM (2003) Reduction of uranium(VI) by mixed iron(II)/iron(III) hydroxide (green rust): formation of UO2 nanoparticles. Environ Sci Technol 37(4):721–727
Li P, Wang J, Wang Y, Liang J, He B, Pan D, Fan Q, Wang X (2019) Photoconversion of U(VI) by TiO2: an efficient strategy for seawater uranium extraction. Chem Eng J 365:231–241
Schulte-Herbrüggen HMA, Semião AJC, Chaurand P, Graham MC (2016) Effect of pH and pressure on uranium removal from drinking water using NF/RO membranes. Environ Sci Technol 50(11):5817–5824
Lu Y (2014) Coordination chemistry in the ocean. Nat Chem 6(3):175–177
Zhou L, Bosscher M, Zhang C, Özçubukçu S, Zhang L, Zhang W, Li CJ, Liu J, Jensen MP, Lai L, He C (2014) A protein engineered to bind uranyl selectively and with femtomolar affinity. Nat Chem 6(3):236–241
Zhang H, Liu W, Li A, Zhang D, Li X, Zhai F, Chen L, Chen L, Wang Y, Wang S (2019) Three mechanisms in one material: uranium capture by a polyoxometalate–organic framework through combined complexation, chemical reduction, and photocatalytic reduction. Angew Chem Int Ed 58(45):16110–16114
Roberts HE, Morris K, Law GTW, Mosselmans JFW, Bots P, Kvashnina K, Shaw S (2017) Uranium(V) incorporation mechanisms and stability in Fe(II)/Fe(III) (oxyhydr) oxides. Environ Sci Technol Lett 4(10):421–426
Stewart BD, Mayes MA, Fendorf S (2010) Impact of uranyl – calcium – carbonato complexes on uranium(VI) adsorption to synthetic and natural sediments. Environ Sci Technol 44(3):928–934
Yang W, Pan Q, Song S, Zhang H (2019) Metal–organic framework-based materials for the recovery of uranium from aqueous solutions. Inorg Chem Front 6(8):1924–1937
Zhao Z, Cheng G, Zhang Y, Han B, Wang X (2021) Metal-organic-framework based functional materials for uranium recovery: performance optimization and structure/functionality-activity relationships. ChemPlusChem 86(8):1177–1192
Song S, Huang Q, Cheng G, Wang W, Lu Z, Zhang R, Wen T, Zhang Y, Wang J, Wang X (2019) Immobilization of U(VI) on hierarchical NiSiO@MgAl and NiSiO@NiAl nanocomposites from wastewater. ACS Sustain Chem Eng 7(3):3475–3486
Zhang S, Yuan D, Zhao J, Ren G, Zhao X, Liu Y, Wang Y, He Y, Ma M, Zhang Q (2021) Highly efficient extraction of uranium from strong HNO3 media achieved on phosphine oxide functionalized superparamagnetic composite polymer microspheres. J Mater Chem A 9(34):18393–18405
Zhao M, Cui Z, Pan D, Fan F, Tang J, Hu Y, Xu Y, Zhang P, Li P, Kong XY, Wu W (2021) An efficient uranium adsorption magnetic platform based on amidoxime-functionalized flower-like Fe3O4@TiO2 core-shell microspheres. ACS Appl Mater Interfaces 13(15):17931–17939
Wang J, Wang Y, Wang W, Ding Z, Geng R, Li P, Pan D, Liang J, Qin H, Fan Q (2020) Tunable mesoporous g-C3N4 nanosheets as a metal-free catalyst for enhanced visible-light-driven photocatalytic reduction of U(VI). Chem Eng J 383:123193
Chen J, Ollis DF, Rulkens WH, Bruning H (1999) Photocatalyzed deposition and concentration of soluble uranium(VI) from TiO2 suspensions. Colloid Surf A-Physicochem Eng Asp 151(1):339–349
Liang P, Yuan L, Du K, Wang L, Li Z, Deng H, Wang X, Luo S-Z, Shi W (2021) Photocatalytic reduction of uranium(VI) under visible light with 2D/1D Ti3C2/CdS. Chem Eng J 420:129831
Li H, Zhai F, Gui D, Wang X, Wu C, Zhang D, Dai X, Deng H, Su X, Diwu J, Lin Z, Chai Z, Wang S (2019) Powerful uranium extraction strategy with combined ligand complexation and photocatalytic reduction by postsynthetically modified photoactive metal-organic frameworks. Appl Catal B 254:47–54
Liang P-l, Yuan L-y, Deng H, Wang X-c, Wang L, Li Z-j, Luo S-z, Shi W-q (2020) Photocatalytic reduction of uranium(VI) by magnetic ZnFe2O4 under visible light. Appl Catal B 267:118688
Li P, Wang J, Wang Y, Dong L, Wang W, Geng R, Ding Z, Luo D, Pan D, Liang J, Fan Q (2021) Ultrafast recovery of aqueous uranium: photocatalytic U(VI) reduction over CdS/g-C3N4. Chem Eng J 425:131552
Chen K, Chen C, Ren X, Alsaedi A, Hayat T (2019) Interaction mechanism between different facet TiO2 and U(VI): experimental and density-functional theory investigation. Chem Eng J 359:944–954
Mühr-Ebert EL, Wagner F, Walther C (2019) Speciation of uranium: compilation of a thermodynamic database and its experimental evaluation using different analytical techniques. Appl Geochem 100:213–222
Amadelli R, Maldotti A, Sostero S, Carassiti V (1991) Photodeposition of uranium oxides onto TiO2 from aqueous uranyl solutions. J Chem Soc Farady Trans 87(19):3267–3273
Wang J, Wang Y, Wang W, Peng T, Liang J, Li P, Pan D, Fan Q, Wu W (2020) Visible light driven Ti3+ self-doped TiO2 for adsorption-photocatalysis of aqueous U(VI). Environ Pollut 262:114373
Le Z, Xiong C, Gong J, Wu X, Pan T, Chen Z, Xie Z (2020) Self-cleaning isotype g-C3N4 heterojunction for efficient photocatalytic reduction of hexavalent uranium under visible light. Environ Pollut 260:114070
Tong X, Wang S, Zuo J, Ge Y, Gao Q, Liu S, Ding J, Liu F, Luo J, Xiong J (2021) Two 2D uranyl coordination complexes showing effective photocatalytic degradation of Rhodamine B and mechanism study. Chin Chem Lett 32(2):604–608
Wang W-D, Bakac A, Espenson JH (1995) Uranium(VI)-catalyzed photooxidation of hydrocarbons with molecular oxygen. Inorg Chem 34(24):6034–6039
Li S, Hu Y, Shen Z, Cai Y, Ji Z, Tan X, Liu Z, Zhao G, Hu S, Wang X (2021) Rapid and selective uranium extraction from aqueous solution under visible light in the absence of solid photocatalyst. Sci China Chem 64(8):1323–1331
Salomone VN, Meichtry JM, Schinelli G, Leyva AG, Litter MI (2014) Photochemical reduction of U(VI) in aqueous solution in the presence of 2-propanol. J Photochem Photobiol A: Chem 277:19–26
Salomone VN, Meichtry JM, Zampieri G, Litter MI (2015) New insights in the heterogeneous photocatalytic removal of U(VI) in aqueous solution in the presence of 2-propanol. Chem Eng J 261:27–35
Burrows HD, Kemp TJ (1974) The photochemistry of the uranyl ion. Chem Soc Rev 3(2):139–165
Mao Y, Bakac A (1996) Photocatalytic Oxidation of Toluene to Benzaldehyde by Molecular Oxygen. J Phys Chem 100(10):4219–4223
Li Y, Zhang G, Eugen Schwarz WH, Li J (2020) Excited-State Chemistry: Photocatalytic Methanol Oxidation by Uranyl@Zeolite through Oxygen-Centered Radicals. Inorg Chem 59(9):6287–6300
Kannan S, Vaughn AE, Weis EM, Barnes CL, Duval PB (2006) Anhydrous Photochemical Uranyl(VI) Reduction: Unprecedented Retention of Equatorial Coordination Accompanying Reversible Axial Oxo/Alkoxide Exchange. J Am Chem Soc 128(43):14024–14025
Xie J, Lin J, Zhou X (2018) pH-dependent microbial reduction of uranium(VI) in carbonate-free solutions: UV-vis, XPS, TEM, and thermodynamic studies. Environ Sci Pollut Res 25(22):22308–22317
Pan Z, Bártová B, LaGrange T, Butorin SM, Hyatt NC, Stennett MC, Kvashnina KO, Bernier-Latmani R (2020) Nanoscale mechanism of UO2 formation through uranium reduction by magnetite. Nat Commun 11(1):4001
Kvashnina KO, Butorin SM, Martin P, Glatzel P (2013) Chemical state of complex uranium oxides. Phys Rev Lett 111(25):253002
Wang Y, Chen Q, Shen X (2016) Preparation of low-temperature sintered UO2 nanomaterials by radiolytic reduction of ammonium uranyl tricarbonate. J Nucl Mater 479:162–166
Li S, Niu Z, Pan D, Cui Z, Shang H, Lian J, Wu W (2022) Efficient photoreduction strategy for uranium immobilization based on graphite carbon nitride/activated carbon nanocomposites. Chin Chem Lett 33(7):3581–3584
Li S, Yang X, Cui Z, Xu Y, Niu Z, Li P, Pan D, Wu W (2021) Efficient photoreduction strategy for uranium immobilization based on graphite carbon nitride/perovskite oxide heterojunction nanocomposites. Appl Catal B 298:120625
Liu Y, Wu S, Liu J, Xie S, Liu Y (2021) Synthesis of g-C3N4/TiO2 nanostructures for enhanced photocatalytic reduction of U(VI) in water. RSC Adv 11(8):4810–4817
Zhang L, Li H, Li L, Deng J, Deng W, Zhao Y (2013) Photocatalytic Reduction of Uranyl Ions over Anatase and Rutile Nanostructured TiO2. Chem Lett 42(7):689–690
Acknowledgements
This work has been supported by the National Natural Science Funds of China (No.12005086) and Fundamental Research Funds for the Central Universities (lzujbky-2020-kb06).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare no competing financial interest.
Additional information
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Cui, Z., Li, S., Wei, X. et al. Photoreduction as an efficient approach for the rapid removal of U(VI) from the aqueous solution. J Radioanal Nucl Chem 331, 4159–4168 (2022). https://doi.org/10.1007/s10967-022-08508-6
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10967-022-08508-6