DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Solvent-driven fractional crystallization for atom-efficient separation of metal salts from permanent magnet leachates

Journal Article · · Nature Communications

Abstract This work reports a dimethyl ether-driven fractional crystallization process for separating rare earth elements and transition metals. The process has been successfully applied in the treatment of rare earth element-bearing permanent magnet leachates as an atom-efficient, reagent-free separation method. Using ~5 bar pressure, the solvent was dissolved into the aqueous system to displace the contained metal salts as solid precipitates. Treatments at distinct temperatures ranging from 20–31 °C enable crystallization of either lanthanide-rich or transition metal-rich products, with single-stage solute recovery of up to 95.9% and a separation factor as high as 704. Separation factors increase with solution purity, suggesting feasibility for eco-friendly solution treatments in series and parallel to purify aqueous material streams. Staged treatments are demonstrated as capable of further improving the separation factor and purity of crystallized products. Upon completion of a crystallization, the solvent can be recovered with high efficiency at ambient pressure. This separation process involves low energy and reagent requirements and does not contribute to waste generation.

Research Organization:
Ames Laboratory (AMES), Ames, IA (United States); Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Sponsoring Organization:
Ames Laboratory; USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Manufacturing Office; USDOE Office of Science (SC)
Grant/Contract Number:
AC02-07CH11358; AC07-05ID14517
OSTI ID:
1874596
Report Number(s):
INL/JOU-22-65588-Rev000; IS-J-10,840; 3789; PII: 31499
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United Kingdom
Language:
English

References (83)

Magnetic Materials and Devices for the 21st Century: Stronger, Lighter, and More Energy Efficient journal December 2010
On the design of crystallization-based separation processes: Review and extension journal January 2006
Solventing out of electrolytes from their aqueous solution journal September 1984
The separation of electrolytes by a “solventing-out” process journal March 1985
Fractional crystallization: Design alternatives and tradeoffs: Fractional Crystallization: Design Alternatives and Tradeoffs journal November 1995
Optimal design of crystallization-based separation schemes journal July 1999
Unified approach for synthesizing crystallization-based separation processes journal July 2000
Atom Economy—A Challenge for Organic Synthesis: Homogeneous Catalysis Leads the Way journal February 1995
The structure of and interactions in binary acetonitrile + water mixtures: Acetonitrile + water mixtures journal December 2012
Separation Hydrometallurgy of Rare Earth Elements book December 2015
Refinement of the crystal structure of Sm2(SO4)3?d8H2O journal January 1976
Energy-saving drying technology for porous media using liquefied DME gas journal April 2008
REE Recovery from End-of-Life NdFeB Permanent Magnet Scrap: A Critical Review journal September 2016
Recovery of Rare-Earth Elements from Neodymium Magnet Waste Using Glycolic, Maleic, and Ascorbic Acids Followed by Solvent Extraction journal December 2018
The preparation of carrier free radiobromine: The separation of KBrO3 and KBr using an organic solvent journal February 1976
Solubility and thermodynamic functions for a 3–2 salt, samarium sulfate, in water and sulfuric acid solutions at temperatures to 350°C journal October 1975
Kinetics of liquid-gas reactions through bubbles journal January 1978
Binary vapor-liquid-liquid equilibrium of dimethyl ether - water and mutual solubilities of methyl chloride and water: Experimental results and data reduction journal December 1988
Diamond nucleation on steel substrates journal March 1993
Systematic separation of a multicomponent mixture of solids based on selective crystallization and dissolution journal January 1991
Developments in the processing and properties of NdFeb-type permanent magnets journal August 2002
Historical overview of silicon crystal pulling development journal April 2000
Simulation study of flat-sheet air gap membrane distillation modules coupled with an evaporative crystallizer for zero liquid discharge water desalination journal September 2016
Efficient separation and high selectivity for nickel from cobalt-solution by a novel chelating resin: Batch, column and competition investigation journal July 2012
Thermodynamics of solvent-driven water extraction from hypersaline brines using dimethyl ether journal April 2022
Removal of heavy metal ions by nanofiltration journal April 2013
Electrodeposition of Dysprosium in pyrrolidinium triflate ionic liquid at ambient temperature: Unraveling system efficiency and impact of solvation interplays on the reduction process journal May 2021
Energy consumption for sugar manufacturing. Part I: Evaporation versus reverse osmosis journal June 2010
Global demand for rare earth resources and strategies for green mining journal October 2016
The solubility of water in mixtures of dimethyl ether and carbon dioxide journal November 2010
Energy-efficient coal dewatering using liquefied dimethyl ether journal August 2010
Recycling of NdFeB magnets using nitration, calcination and water leaching for REE recovery journal January 2017
Mathematical modelling and analysis of an industrial scale evaporative crystallizer producing lactose monohydrate journal June 2015
Dimethyl ether (DME) as an alternative fuel journal June 2006
A critical review on solvent extraction of rare earths from aqueous solutions journal February 2014
Modeling solution vapor equilibria with solvation and solute assembly journal August 2021
Idaho database of solution thermodynamics journal September 2021
Applying design of experiments to evaluate economic feasibility of rare-earth element recovery journal January 2020
Techno-economic Assessment of a Novel SmCo Permanent Magnet Manufacturing Method journal January 2021
Comparative life cycle analysis for value recovery of precious metals and rare earth elements from electronic waste journal October 2019
Separation of valuable elements from NiMH battery leach liquor via antisolvent precipitation journal March 2020
Solvent extraction of lithium ions using benzoyltrifluoroacetone in new solvents journal January 2021
Bridging Hydrometallurgy and Biochemistry: A Protein-Based Process for Recovery and Separation of Rare Earth Elements journal October 2021
Sustainable Recycling of Rare-Earth Elements from NdFeB Magnet Swarf: Techno-Economic and Environmental Perspectives journal November 2021
Water Interplays during Dysprosium Electrodeposition in Pyrrolidinium Ionic Liquid: Deconvoluting the Pros and Cons for Rare Earth Metallization journal October 2021
Techno-economic and Life Cycle Analysis for Bioleaching Rare-Earth Elements from Waste Materials journal December 2017
Metal Recovery from Spent Samarium–Cobalt Magnets Using a Trichloride Ionic Liquid journal December 2018
Sustainable Urban Mining of Critical Elements from Magnet and Electronic Wastes journal November 2019
On Inventing Reactions for Atom Economy journal September 2002
Process designs for fractional crystallization from solution journal September 1993
Fractional Precipitation or Crystallization Systems - Efficiency of Fractionation journal October 1955
How to Design Fractional Crystallization Processes journal December 1970
The Heat of Hydration of Cobalt Sulfate Hexahydrate to Heptahydrate. Their Solubilities and Heats of Solution 1 journal April 1965
Viscosity of Aqueous NaCl Solutions with Dissolved CO 2 at (30 to 60) °C and (10 to 20) MPa journal August 2004
Selective sulfidation of metal compounds journal December 2021
Examining different recycling processes for lithium-ion batteries journal February 2019
Mass action model of solution activity via speciation by solvation and ion pairing equilibria journal November 2021
Retention of single crystals of two Co( ii ) complexes during chemical reactions and rearrangement journal January 2014
Recycling of rare earths from NdFeB magnets using a combined leaching/extraction system based on the acidity and thermomorphism of the ionic liquid [Hbet][Tf 2 N] journal January 2015
Recovery of rare earth elements with ionic liquids journal January 2017
Selective electrochemical extraction of REEs from NdFeB magnet waste at room temperature journal January 2018
Crystallization kinetics of Na 2 CO 3 in Bayer aluminate solutions during the evaporation process journal January 2018
Rationally designed rare earth separation by selective oxalate solubilization journal January 2020
Solute displacement in the aqueous phase of water–NaCl–organic ternary mixtures relevant to solvent-driven water treatment journal January 2020
Impact of process parameters on product size and morphology in hydrometallurgical antisolvent crystallization journal January 2022
Removal of transition metals from rare earths by solvent extraction with an undiluted phosphonium ionic liquid: separations relevant to rare-earth magnet recycling journal January 2013
The Separation of Electrolytes in Aqueous Solution by Miscible Organic Solvents journal February 1979
Separation of the System NaCl-NaBr-Nal by “Solventing Out” from Aqueous Solution journal May 1983
Extraction behavior of selected rare earth metals from acidic chloride media using tetrabutyl diglycolamide journal September 2017
Recovery of rare earth elements from acid mine drainage by ion exchange journal January 2020
Rare Earth Elements Recovery from Waste Fluorescent Lamps: A Review journal December 2014
The crystal structure of cobalt sulfate hexahydrate journal December 1962
On the crystal chemistry of salt hydrates. III. The determination of the crystal structure of FeSO 4 .7H 2 O (melanterite) journal September 1964
Optimization design of cane sugar evaporative crystallizer based on orthogonal test and computational fluid dynamics journal April 2020
Challenges in Metal Recycling journal August 2012
Toward a sustainable materials system journal June 2018
Rare earth elements: Mendeleev’s bane, modern marvels journal January 2019
Rare Earths: Market Disruption, Innovation, and Global Supply Chains journal November 2016
Hydrometallurgical Recovery of Rare Earth Elements from NdFeB Permanent Magnet Scrap: A Review journal June 2020
Leaching and Recovery of Rare-Earth Elements from Neodymium Magnet Waste Using Organic Acids journal September 2018
Scandium Recovery from an Ammonium Fluoride Strip Liquor by Anti-Solvent Crystallization journal September 2018
Recent advances in acid-free dissolution and separation of rare earth elements from the magnet waste journal January 2021
Compilation of Henry's law constants (version 4.0) for water as solvent journal January 2015