Synergistic Effect of Core/Shell-Structured Composite Fibers: Efficient Recovery of Rare-Earth Elements from Spent NdFeB Permanent Magnets

Youngkyun Jung, Yun Lee, Su-Jin Yoon, Jae-Woo Choi

Advanced Fiber Materials ›› 2024, Vol. 6 ›› Issue (6) : 1729-1745.

Advanced Fiber Materials ›› 2024, Vol. 6 ›› Issue (6) : 1729-1745. DOI: 10.1007/s42765-024-00442-4
Research Article

Synergistic Effect of Core/Shell-Structured Composite Fibers: Efficient Recovery of Rare-Earth Elements from Spent NdFeB Permanent Magnets

Author information +
History +

Abstract

NdFeB magnets are third-generation permanent magnets that are employed as indispensable components in various industries. Notably, rare-earth elements (REEs) such as Dy and Nd must be efficiently recovered from end-of-life magnets to enable resource circulation and reinforce unstable supply chains. To that end, this paper reports synergistically performing core/shell-structured composite fibers (CSCFs) containing sodium polyacrylate and nanoporous zeolitic imidazolate framework-8 (NPZIF-8) nanocrystals as a readily recoverable adsorbent with an exceptional REE-adsorbing ability. The CSCF core forms an NPZIF-8 nanocrystal shell on the fiber surface as well as draws REEs using its dense sodium carboxylate groups into the NPZIF-8 nanocrystal lattice with high specific surface area. The CSCFs exhibit significantly higher maximum adsorption capacities (468.60 and 435.13 mg·g−1) and kinetic rate constants (2.02 and 1.92 min−1) for the Nd3+ and Dy3+ REEs than those of previously reported REE adsorbents. Additionally, the simple application of the CSCFs to an adsorption reactor considerably mitigates the adsorbent-shape-induced pressure drop, thereby directly influencing the energy efficiency of the recovery. Moreover, the high REE-recovery ability, tractability, and recyclability of the CSCFs offers a pragmatic pathway to achieving cost-effective REE recovery. Overall, this study provides new insights into designing synergistically performing core/shell architectures for feasible REE recovery.

Graphical Abstract

Cite this article

Download citation ▾
Youngkyun Jung, Yun Lee, Su-Jin Yoon, Jae-Woo Choi. Synergistic Effect of Core/Shell-Structured Composite Fibers: Efficient Recovery of Rare-Earth Elements from Spent NdFeB Permanent Magnets. Advanced Fiber Materials, 2024, 6(6): 1729‒1745 https://doi.org/10.1007/s42765-024-00442-4

References

[1.]
ZhangY, YanJ, XuJ, TianC, MatyjaszewskiK, TiltonRD, LowryGV. Phosphate polymer nanogel for selective and efficient rare earth element recovery. Environ Sci Technol, 2021, 55: 12549
CrossRef Google scholar
[2.]
ZhouF, XiaoY, GuoM, TangY, ZhangW, QiuR. Selective leaching of rare earth elements from ion-adsorption rare earth tailings: a synergy between CeO2 reduction and Fe/Mn stabilization. Environ Sci Technol, 2021, 55: 11328
CrossRef Google scholar
[3.]
DwadasiBS, GuptaS, DawareS, Goverapet SrinivasanS, RaiB. Differential stabilization of the metal–ligand complexes between organic and aqueous phases drives the selectivity of phosphoric acid ligands toward heavier rare earth elements. Ind Eng Chem Res, 2018, 57: 17209
CrossRef Google scholar
[4.]
YangY, WaltonA, SheridanR, GüthK, GaußR, GutfleischO, BuchertM, SteenariB-M, Van GervenT, JonesPT. REE recovery from end-of-life NdFeB permanent magnet scrap: a critical review. J Sustain Metall, 2017, 3: 122
CrossRef Google scholar
[5.]
BinnemansK, McGuinessP, JonesPT. Rare-earth recycling needs market intervention. Nat Rev Mater, 2021, 6: 459
CrossRef Google scholar
[6.]
IftekharS, HeidariG, AmanatN, ZareEN, AsifMB, HassanpourM, LehtoVP, SillanpaaM. Porous materials for the recovery of rare earth elements, platinum group metals, and other valuable metals: a review. Environ Chem Lett, 2022, 20: 3697
CrossRef Google scholar
[7.]
JinH, AfiunyP, DoveS, FurlanG, ZakotnikM, YihY, SutherlandJW. Life cycle assessment of neodymium–iron–boron magnet-to-magnet recycling for electric vehicle motors. Environ Sci Technol, 2018, 52: 3796
CrossRef Google scholar
[8.]
LorenzT, BertauM. Recycling of rare earth elements from FeNdB-magnets via solid-state chlorination. J Clean Prod, 2019, 215: 131
CrossRef Google scholar
[9.]
VenkatesanP, HoogerstraeteTV, HennebelT, BinnemansK, SietsmaJ, YangY. Selective electrochemical extraction of REEs from NdFeB magnet waste at room temperature. Green Chem, 2018, 20: 1065
CrossRef Google scholar
[10.]
KapustkaK, ZiegmannG, Klimecka-TatarD. Technological and ecological safety in aspect of chemical properties of recycled neodymium magnets—electric motors and hard disk. Prod Eng Arch, 2017, 17: 36
CrossRef Google scholar
[11.]
BianY, GuoS, JiangL, TangK, DingW. Extraction of rare earth elements from permanent magnet scraps by FeO–B2O3 flux treatment. J Sustain Metall, 2015, 1: 151
CrossRef Google scholar
[12.]
SaitoT, SatoH, OzawaS, YuJ, MotegiT. The extraction of Nd from waste Nd–Fe–B alloys by the glass slag method. J Alloys Compd, 2003, 353: 189
CrossRef Google scholar
[13.]
KumariA, JhaMK, PathakDD. An innovative environmental process for the treatment of scrap Nd–Fe–B magnets. J Environ Manag, 2020, 273 111063
CrossRef Google scholar
[14.]
LiuF, PorvaliA, WangJ, WangH, PengC, WilsonBP, LundströmM. Recovery and separation of rare earths and boron from spent Nd–Fe–B magnets. Miner Eng, 2020, 145 106097
CrossRef Google scholar
[15.]
RhoB-J, SunP-P, ChoS-Y. Recovery of neodymium and praseodymium from nitrate-based leachate of permanent magnet by solvent extraction with trioctylphosphine oxide. Sep Purif Technol, 2020, 238 116429
CrossRef Google scholar
[16.]
OreficeM, BinnemansK. Solvometallurgical process for the recovery of rare-earth elements from Nd–Fe–B magnets. Sep Purif Technol, 2021, 258 117800
CrossRef Google scholar
[17.]
ItohM, MiuraK, MachidaK-I. Novel rare earth recovery process on Nd–Fe–B magnet scrap by selective chlorination using NH4Cl. J Alloys Compd, 2009, 477: 484
CrossRef Google scholar
[18.]
JungY, DoT, ChoiUS, JungK-W, ChoiJ-W. Cage-like amine-rich polymeric capsule with internal 3D center-radial channels for efficient and selective gold recovery. Chem Eng J, 2022, 438 135618
CrossRef Google scholar
[19.]
DingA, LiuC, ZhangX, LeiL, XiaoC. ZnCl2: a green brønsted acid for selectively recovering rare earth elements from spent NdFeB permanent magnets. Environ Sci Technol, 2022, 56: 4404
CrossRef Google scholar
[20.]
XuX, SturmS, SamardzijaZ, ScancarJ, MarkovicK, RozmanKZ. A facile method for the simultaneous recovery of rare-earth elements and transition metals from Nd–Fe–B magnets. Green Chem, 2020, 22: 1105
CrossRef Google scholar
[21.]
HuaZ, WangJ, WangL, ZhaoZ, LiX, XiaoY, YangY. Selective extraction of rare earth elements from NdFeB scrap by molten chlorides. ACS Sustain Chem Eng, 2014, 2: 2536
CrossRef Google scholar
[22.]
OkabeTH, TakedaO, FukudaK, UmetsuY. Direct extraction and recovery of neodymium metal from magnet scrap. Mater Trans, 2003, 44: 798
CrossRef Google scholar
[23.]
KimD, PowellLE, DelmauLH, PetersonES, HerchenroederJ, BhaveRR. Selective extraction of rare earth elements from permanent magnet scraps with membrane solvent extraction. Environ Sci Technol, 2015, 49: 9452
CrossRef Google scholar
[24.]
DeshmaneVG, IslamSZ, BhaveRR. Selective recovery of rare earth elements from a wide range of e-waste and process scalability of membrane solvent extraction. Environ Sci Technol, 2019, 54: 550
CrossRef Google scholar
[25.]
Ni’amAC, LiuY-H, WangY-F, ChenS-W, ChangG-M, YouS-J. Recovery of neodymium from waste permanent magnets by hydrometallurgy using hollow fibre supported liquid membranes. Solvent Extr Res Dev Jpn, 2020, 27: 69
CrossRef Google scholar
[26.]
DongZ, MattocksJA, DeblondeGJ-P, HuD, JiaoY, CotruvoJA Jr, ParkDM. Bridging hydrometallurgy and biochemistry: a protein-based process for recovery and separation of rare earth elements. ACS Cent Sci, 2021, 7: 1798
CrossRef Google scholar
[27.]
de VargasBG, da SilvaMG, VieiraMGA. Adsorption potential for the concentration and recovery of rare earth metals from NdFeB magnet scrap in the hydrometallurgical route: a review in a circular economy approach. J Clean Prod, 2022, 380 135112
CrossRef Google scholar
[28.]
OuyangD, ZhuoY, HuL, ZengQ, HuY, HeZ. Research on the adsorption behavior of heavy metal ions by porous material prepared with silicate tailings. Minerals, 2019, 9: 291
CrossRef Google scholar
[29.]
KavunV, van der VeenMA, RepoE. Selective recovery and separation of rare earth elements by organophosphorus modified MIL-101 (Cr). Microporous Mesoporous Mater, 2021, 312 110747
CrossRef Google scholar
[30.]
ZhangM, YangK, CuiJ, YuH, WangY, ShanW, LouZ, XiongY. 3D-agaric like core–shell architecture UiO-66-NH2@ZIF-8 with robust stability for highly efficient REEs recovery. Chem Eng J, 2020, 386 124023
CrossRef Google scholar
[31.]
JiangL, ZhangW, LuoC, ChengD, ZhuJ. Adsorption toward trivalent rare earth element from aqueous solution by zeolitic imidazolate frameworks. Ind Eng Chem Res, 2016, 55: 6365
CrossRef Google scholar
[32.]
IeamviteevanichP, PalapornD, ChanlekN, Poo-arpornY, MongkolthanarukW, EichhornSJ, PinitsoontornS. Carbon nanofiber aerogel/magnetic core–shell nanoparticle composites as recyclable oil sorbents. ACS Appl Nano Mater, 2020, 3: 3939
CrossRef Google scholar
[33.]
HaghdoostF, BahramiSH, BarzinJ, GhaeeA. Preparation and characterization of electrospun polyethersulfone/polyvinylpyrrolidone-zeolite core–shell composite nanofibers for creatinine adsorption. Sep Purif Technol, 2021, 257 117881
CrossRef Google scholar
[34.]
YiR, YeG, ChenJ. Synthesis of core–shell magnetic titanate nanofibers composite for the efficient removal of Sr(II). RSC Adv, 2019, 9: 27242
CrossRef Google scholar
[35.]
JungY, KoYG, DoT, ChunY, ChoiUS, KimCH. Core/shell hybrid fiber with aminated PAN and Fe2O3 as a high-capacity adsorbent for phosphate ions. J Hazard Mater, 2019, 378 120726
CrossRef Google scholar
[36.]
IeamviteevanichP, MongkolthanarukW, FaungnawakijK, DaneshvarE, BhatnagarA, PinitsoontornS. Nanoporous magnetic carbon nanofiber aerogels with embedded α-Fe/γ-Fe core–shell nanoparticles for oil sorption and recovery. ACS Appl Nano Mater, 2022, 5: 2885
CrossRef Google scholar
[37.]
YangJ, TongM, HanG, ChangM, YanT, YingY, YangQ, LiuD. Solubility-boosted molecular sieving-based separation for purification of acetylene in core–shell IL@ MOF composites. Adv Funct Mater, 2023, 33: 2213743
CrossRef Google scholar
[38.]
PhamT-D, TruongT-T-T, NguyenH-L, HoangL-B-L, BuiV-P, TranT-T-M, DinhT-D, LeT-D. Synthesis and characterization of novel core–shell ZnO@SiO2 nanoparticles and application in antibiotic and bacteria removal. ACS Omega, 2022, 7: 42073
CrossRef Google scholar
[39.]
VenkatesanP, Vander HoogerstraeteT, HennebelT, SietsmaJ, YangY. Selective electrochemical extraction of REEs from NdFeB magnet waste at room temperature. Green Chem, 2018, 20: 1065
CrossRef Google scholar
[40.]
LinH-C, HongJ-L. Metalized polyacrylates as efficient binder for a sulfurized polyacrylonitrile/polydopamine active material in sulfur cathodes for room temperature sodium–sulfur batteries. ACS Appl Energ Mater, 2022, 5: 11304
CrossRef Google scholar
[41.]
JungY, KoYG, NahIW, ChoiUS. Designing large-sized and spherical CO2 adsorbents for highly reversible CO2 capture and low pressure drop. Chem Eng J, 2022, 427 131781
CrossRef Google scholar
[42.]
Delgado-MelladoN, LarribaM, NavarroP, RigualV, AyusoM, GarcíaJ, RodríguezF. Thermal stability of choline chloride deep eutectic solvents by TGA/FTIR-ATR analysis. J Mol Liq, 2018, 260: 37
CrossRef Google scholar
[43.]
GongH, IlavskyJ, KuzmenkoI, ChenS, YanH, CooperCB, ChenG, ChenY, ChiongJA, JiangY. Formation mechanism of flower-like polyacrylonitrile particles. J Am Chem Soc, 2022, 144: 17576
CrossRef Google scholar
[44.]
LiG, XiaoJ, ZhangW. Efficient and reusable amine-functionalized polyacrylonitrile fiber catalysts for Knoevenagel condensation in water. Green Chem, 2012, 14: 2234
CrossRef Google scholar
[45.]
RahamanMSA, IsmailAF, MustafaA. A review of heat treatment on polyacrylonitrile fiber. Polym Degrad Stab, 2007, 92: 1421
CrossRef Google scholar
[46.]
ZengJ, WangQ, ShiY, LiuP, ChenR. Osmotic pumping and salt rejection by polyelectrolyte hydrogel for continuous solar desalination. Adv Energy Mater, 2019, 9: 1900552
CrossRef Google scholar
[47.]
SunL, LiuY, LuoB, YanF, LiuX, ZhuF, ShiW. Hierarchical multiphase (Ni, Co)-Se with adjustable interlayer distance derived from reconstructed ZIF-L for enhanced hybrid-supercapacitors. Chem Eng J, 2023, 454 140088
CrossRef Google scholar
[48.]
JeonC, HöllWH. Chemical modification of chitosan and equilibrium study for mercury ion removal. Water Res, 2003, 37: 4770
CrossRef Google scholar
[49.]
GergoricM, BarrierA, ReteganT. Recovery of rare-earth elements from neodymium magnet waste using glyclic, maleic, and ascorbic acids followed by solvent extraction. J Sustain Matall, 2019, 5: 85
CrossRef Google scholar
[50.]
LeeEY, WongSY, PhangSJ, WongV-L, CheahKH. Additively manufactured photoreactor with immobilized thermoset acrylic-graphitic carbon nitride nanosheets for water remediation: Response surface methods and adsorption modelling studies. Chem Eng J, 2023, 455 140633
CrossRef Google scholar
[51.]
JiangL, DuanJ, ZhuJ, ChenS, AntoniettiM. Iron-cluster-directed synthesis of 2D/2D Fe–N–C/MXene superlattice-like heterostructure with enhanced oxygen reduction electrocatalysis. ACS Nano, 2020, 14: 2436
CrossRef Google scholar
[52.]
XieW, GaoC, LiJ. Sustainable biodiesel production from low-quantity oils utilizing H6PV3MoW8O40 supported on magnetic Fe3O4/ZIF-8 composites. Renew Energy, 2021, 168: 927
CrossRef Google scholar
[53.]
WangW, XuJ, WangA. A pH-, salt- and solvent-responsive carboxymethylcellulose-g-poly (sodium acrylate)/medical stone superabsorbent composite with enhanced swelling and responsive properties. Express Polym Lett, 2011, 5: 385
CrossRef Google scholar
[54.]
GuanX-H, ChenG-H, ShangC. ATR-FTIR and XPS study on the structure of complexes formed upon the adsorption of simple organic acids on aluminum hydroxide. J Environ Sci, 2007, 19: 438
CrossRef Google scholar
[55.]
MaanO, SongP, ChenN, LuQ. An in situ procedure for the preparation of zeolitic imidazolate framework-8 polyacrylamide hydrogel for adsorption of aqueous pollutants. Adv Mater Interfaces, 2019, 6: 1801895
CrossRef Google scholar
[56.]
NayakS, KumalRR, LeeSE, UysalA. Elucidating trivalent ion adsorption at floating carboxylic acid monolayers: charge reversal or water reorganization?. J Phys Chem Lett, 2023, 14: 3685
CrossRef Google scholar
[57.]
SartorettiE, NovaraC, ChiodoniA, GiorgisF, PiumettiM, BensaidS, RussoN, FinoD. Nanostructured ceria-based catalysts doped with La and Nd: how acid-base sites and redox properties determine the oxidation mechanisms. Catal Today, 2022, 390: 117
CrossRef Google scholar
[58.]
TalikE, KruczekM, SakowskaH, UjmaZ, GałaM, NeumannM. XPS characterisation of neodymium gallate wafers. J Alloys Compd, 2004, 377: 259
CrossRef Google scholar
[59.]
IwanowskiR, HeinonenM, PrackaI, KachniarzJ. XPS characterization of single crystalline SrLaGa3O7: Nd. Appl Surf Sci, 2013, 283: 168
CrossRef Google scholar
[60.]
KohikiS, HayashiS, AdachiH, HattaS-I, SetsuneK, WasaK. Electron spectroscopy of Nd2 xCexCuO4 y (x = 0, 015, and 023) thin films. J Phys Soc Jpn, 1989, 58: 4139
CrossRef Google scholar
[61.]
RalkhalS, ShahrabiT, RamezanzadehB. Synthesis and construction of a highly potent hybrid organic/inorganic anti-corrosive pigment for effective corrosion control of mild steel in simulated seawater. Constr Build Mater, 2019, 222: 400
CrossRef Google scholar
[62.]
AhmadZU, YaoL, WangJ, GangDD, IslamF, LianQ, ZappiME. Neodymium embedded ordered mesoporous carbon (OMC) for enhanced adsorption of sunset yellow: characterizations, adsorption study and adsorption mechanism. Chem Eng J, 2019, 359: 814
CrossRef Google scholar
[63.]
TholkappiyanR, VishistaK. Tuning the composition and magnetostructure of dysprosium iron garnets by co-substitution: an XRD, FT-IR, XPS and VSM study. Appl Surf Sci, 2015, 351: 1016
CrossRef Google scholar
[64.]
RekhaG, TholkappiyanR, VishistaK, HamedF. Systematic study on surface and magnetostructural changes in Mn-substituted dysprosium ferrite by hydrothermal method. Appl Surf Sci, 2016, 385: 171
CrossRef Google scholar
[65.]
D’AngeloP, ZitoloA, MiglioratiV, ChillemiG, DuvailM, VitorgeP, AbadieS, SpeziaR. Revised ionic radii of lanthanoid(III) ions in aqueous solution. Inorg Chem, 2011, 50: 4572
CrossRef Google scholar
[66.]
JinH, AfiunyP, McIntyreT, YihY, SutherlandJW. Comparative life cycle assessment of NdFeB magnets: virgin production versus magnet-to-magnet recycling. Procedia CIRP, 2016, 48: 45
CrossRef Google scholar
[67.]
MünchenDD, VeitHM. Neodymium as the main feature of permanent magnets from hard disk drives (HDDs). Waste Manag, 2017, 61: 372
CrossRef Google scholar
[68.]
Ni'amAC, WangY-F, ChenS-W, YouS-J. Recovery of rare earth elements from waste permanent magnet (WPMs) via selective leaching using the Taguchi method. J Taiwan Inst Chem Eng, 2019, 97: 137
CrossRef Google scholar
[69.]
LiuZ, WuJ, LiuX, WangW, LiZ, XuR, DingY, WangJ. Recovery of neodymium, dysprosium, and cobalt from NdFeB magnet leachate using an unsymmetrical dialkylphosphinic acid extractant, INET-3. J Rare Earths, 2020, 38: 1114
CrossRef Google scholar
[70.]
BorosE, HollandJP. Chemical aspects of metal ion chelation in the synthesis and application antibody-based radiotracers. J Label Compd Radiopharm, 2018, 61: 652
CrossRef Google scholar
[71.]
LiB, ZhangY, MaD, ShiZ, MaS. Mercury nano-trap for effective and efficient removal of mercury(II) from aqueous solution. Nat Commun, 2014, 5: 5537
CrossRef Google scholar
[72.]
AiK, RuanC, ShenM, LuL. MoS2 nanosheets with widened interlayer spacing for high-efficiency removal of mercury in aquatic systems. Adv Funct Mater, 2016, 26: 5542
CrossRef Google scholar
[73.]
RiañoS, BinnemansK. Extraction and separation of neodymium and dysprosium from used NdFeB magnets: an application of ionic liquids in solvent extraction towards the recycling of magnets. Green Chem, 2015, 17: 2931
CrossRef Google scholar
[74.]
YamadaE, MurakamiH, NishihamaS, YoshizukaK. Separation process of dysprosium and neodymium from waste neodymium magnet. Sep Purif Technol, 2018, 192: 62
CrossRef Google scholar
Funding
National Research Foundation of Korea(2020M3H4A3106366)

Accesses

Citations

Detail

Sections
Recommended

/