Rare-earth recycling using a functionalized ionic liquid for the selective dissolution and revalorization of Y2O3:Eu3+ from lamp phosphor waste

Dupont, David; Binnemans, Koen

doi:10.1039/c4gc02107j

Cited by 198 publications

(184 citation statements)

References 55 publications

(120 reference statements)

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“…solvent-, and waste-intensive liquid-liquid extraction steps to purify the individual REs (29). Therefore, recycling of REs from phosphor waste could equally benefit from, simpler, more efficient separations techniques.…”

Section: Significancementioning

confidence: 99%

“…Lamp phosphor waste consists of the non-RE-containing halophosphate, (Sr,Ca) 10 (29). Of these, YOX has the highest intrinsic value because it contains 80 wt % of the total RE content of the phosphor waste and is composed exclusively of the two critical RE elements, Y and Eu.…”

mentioning

confidence: 99%

“…Of these, YOX has the highest intrinsic value because it contains 80 wt % of the total RE content of the phosphor waste and is composed exclusively of the two critical RE elements, Y and Eu. Recent developments in the recycling of phosphor materials have largely focused on the recovery of Eu and Y from YOX (11,(30)(31)(32)(33)(34)(35)(36)(37)(38) (29). Currently, however, only one industrially applied recycling process exists for lamp phosphor waste (29,39).…”

mentioning

confidence: 99%

“…Dupont and Binnemans recently reported on the selective dissolution of YOX and recovery of yttrium and europium using the functionalized ionic liquid betainium bis(trifluoromethylsulfonyl)imide, [Hbet][Tf 2 N] (29). Currently, however, only one industrially applied recycling process exists for lamp phosphor waste (29,39). Solvent extraction of the resulting Eu-and Y-containing concentrates provides high-purity, recycled materials.…”

mentioning

confidence: 99%

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Accomplishing simple, solubility-based separations of rare earth elements with complexes bearing size-sensitive molecular apertures

Bogart

Cole

Boreen

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

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Rare earth (RE) metals are critical components of electronic materials and permanent magnets. Recycling of consumer materials is a promising new source of rare REs. To incentivize recycling, there is a clear need for the development of simple methods for targeted separations of mixtures of RE metal salts. Metal complexes of a tripodal hydroxylaminato ligand, TriNOx 3-, featured a size-sensitive aperture formed of its three η 2 -(N,O) ligand arms. Exposure of cations in the aperture induced a self-associative equilibrium comprising RE(TriNOx)THF and [RE(TriNOx)] 2 species. Differences in the equilibrium constants K dimer for early and late metals enabled simple separations through leaching. Separations were performed on RE1/RE2 mixtures, where RE1 = La-Sm and RE2 = Gd-Lu, with emphasis on Eu/Y separations for potential applications in the recycling of phosphor waste from compact fluorescent light bulbs. Using the leaching method, separations factors approaching 2,000 were obtained for early-late RE combinations. Following solvent optimization, >95% pure samples of Eu were obtained with a 67% recovery for the technologically relevant Eu/Y separation. (11)(12)(13)(14). Limitations associated with their beneficiation and separations, especially their solvent-, waste-, and energy intensities, have contributed to the concentration of suppliers in the People's Republic of China. Supply risks for these elements have emerged, particularly in the face of current and growing demand in the next 20 y (15, 16). Because the global marketplace for these elements is dominated by a single source (17), prices for primary rare earth (RE) materials are volatile (18). As a result, the US Department of Energy has classified many of these elements as "critical" (19). There is a clear need to find potential new supplies of these elements.Recent life cycle assessments have indicated that recycling of consumer materials is a promising alternative to conventional production processes (20). Despite this assertion, as recently as 2011, less than 1% of RE-containing materials were being recycled (21). These low recycling rates stem from a combination of sporadic collection procedures and lack of efficient separations and preprocessing steps (22)(23)(24)(25)(26)(27).To contribute to incentivizing the "urban mining" of REcontaining materials, we recently initiated efforts toward new, simplified methods in RE separations (28). Our initial work focused on the separation of neodymium (Nd) and dysprosium (Dy), two key components of neomagnets (Nd 2 Fe 14 B). We disclosed the development of the tripodal nitroxide ligand, [((2-t BuNO)C 6 H 4 CH 2 ) 3 N] 3− (TriNOx 3-), which induced a selfassociation equilibrium between monomeric Nd(TriNOx)THF/ dimeric [Nd(TriNOx)] 2 species. The position of this equilibrium was found to be strongly dependent on the size of the RE cation. We showed proof of concept that differences in the self-association equilibrium constants between Nd and Dy could be exploited to achieve 95% pure materials through a simple leachi...

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Section: Significancementioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

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Accomplishing simple, solubility-based separations of rare earth elements with complexes bearing size-sensitive molecular apertures

Bogart

Cole

Boreen

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

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“…that can be adjusted by varying either the anion or the cation to achieve applications that are credible alternatives to conventional solvents for the extraction, separation and purification of metals and metal oxides [5][6][7][8][9][10]. A series of publications from Binneman's and Nockemann's research groups [6,[11][12][13][14][15][16] using betaine as an extractant [12,13], and in the recovery of europium (Eu) and yttrium (Y) from lamp phosphor waste powders [14]. The solubility of the rare earth oxides in…”

Section: Introductionmentioning

confidence: 99%

Interactions between trivalent rare earth oxides and mixed [Hbet][Tf2N]:H2O systems in the development of a one-step process for the separation of light from heavy rare earth elements

Schaeffer

Grimes

Cheeseman

2016

Inorganica Chimica Acta

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Identification of lanthanum‐specific peptides for future recycling of rare earth elements from compact fluorescent lamps

Lederer

Curtis

Bachmann

et al. 2017

Biotech & Bioengineering

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As components of electronic scrap, rare earth minerals are an interesting but little used source of raw materials that are highly important for the recycling industry. Currently, there exists no cost-efficient technology to separate rare earth minerals from an electronic scrap mixture. In this study, phage surface display has been used as a key method to develop peptides with high specificity for particular inorganic targets in electronic scrap. Lanthanum phosphate doped with cerium and terbium as part of the fluorescent phosphors of spent compact fluorescent lamps (CFL) was used as a target material of economic interest to test the suitability of the phage display method to the separation of rare earth minerals. One random pVIII phage library was screened for peptide sequences that bind specifically to the fluorescent phosphor LaPO :Ce ,Tb (LAP). The library contained at least 100 binding pVIII peptides per phage particle with a diversity of 1 × 10 different phage per library. After three rounds of enrichment, a phage clone containing the surface peptide loop RCQYPLCS was found to bind specifically to LAP. Specificity and affinity of the identified phage bound peptide was confirmed by using binding and competition assays, immunofluorescence assays, and zeta potential measurements. Binding and immunofluorescence assays identified the peptide's affinity for the fluorescent phosphor components CAT (CeMgAl O :Tb ) and BAM (BaMgAl O :Eu ). No affinity was found for other fluorescent phosphor components such as YOX (Y O :Eu ). The binding specificity of the RCQYPLCS peptide loop was improved 3-51-fold by using alanine scanning mutagenesis. The identification of peptides with high specificity and affinity for special components in the fluorescent phosphor in CFLs provides a potentially new strategic approach to rare earth recycling. Biotechnol. Bioeng. 2017;114: 1016-1024. © 2016 Wiley Periodicals, Inc.

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Rare-earth recycling using a functionalized ionic liquid for the selective dissolution and revalorization of Y₂O₃:Eu³⁺ from lamp phosphor waste

Abstract: A recycling process for lamp phosphor waste has been developed based on the selective dissolution and revalorization of the valuable red lamp phosphor Y2O3:Eu3+ in the functionalized ionic liquid [Hbet][Tf2N].

Cited by 198 publications

References 55 publications

Accomplishing simple, solubility-based separations of rare earth elements with complexes bearing size-sensitive molecular apertures

Accomplishing simple, solubility-based separations of rare earth elements with complexes bearing size-sensitive molecular apertures

Interactions between trivalent rare earth oxides and mixed [Hbet][Tf2N]:H2O systems in the development of a one-step process for the separation of light from heavy rare earth elements

Identification of lanthanum‐specific peptides for future recycling of rare earth elements from compact fluorescent lamps

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