Recycling of rare earths: a critical review

The rare-earth elements (REEs) are becoming increasingly important in the transition to a green economy, due to their essential role in permanent magnets, lamp phosphors, catalysts, rechargeable batteries etc. With China presently producing more than 90% of the global REE output and its increasingly tight export quota, the rest of the world is confronted with a REE supply risk. Mining companies are now actively seeking new exploitable REE deposits while some old mines are being reopened. Because of the absence of economical and/or operational primary deposits on their territory, many countries will have to rely on recycling of REEs from pre-consumer scrap, industrial residues and REE-containing End-of-Life products. REE recycling is also recommended in view of the so-called “balance problem”. For instance, primary mining of REE ores for neodymium generates an excess of the more abundant elements, lanthanum and cerium. Therefore, recycling of neodymium can reduce the total amount of REE ores that need to be extracted. Despite a vast, mostly lab-scale research effort on REE recycling, up to 2011 less than 1% of the REEs were actually recycled. This is mainly due to inefficient collection, technological problems and, especially, a lack of incentives. A drastic improvement in the recycling of REEs is, therefore, an absolute necessity. This can only be realized by developing efficient, fully integrated recycling routes, which can take advantage of the rich REE recycling literature. This paper provides an overview of this literature, with emphasis on three main applications: permanent magnets, nickel metal hydride batteries and lamp phosphors. The state of the art in preprocessing of End-of-Life materials containing REEs and the final REE recovery is discussed in detail. Both pyrometallurgical and hydrometallurgical routes for REE separation from non-REE elements in the recycled fractions are reviewed. The relevance of Life Cycle Assessment (LCA) for REE recycling is emphasized. The review corroborates that, in addition to mitigating the supply risk, REE recycling can reduce the environmental challenges associated with REE mining and processing.

[1]  Masahiro Masuda,et al.  Effective Recovery of Nd–Fe–B Sintered Magnet Scrap Powders as Isotropic Bonded Magnets , 2003 .

[2]  C. A. Morais,et al.  Study of the recovery of rare earth elements from computer monitor scraps – Leaching experiments , 2010 .

[3]  Hironori Sato,et al.  Extraction of Rare Earth from La–Ni Alloys by the Glass Slag Method , 2003 .

[4]  Hideaki Itoh,et al.  Resource recovery from NdFeB sintered magnet by hydrothermal treatment , 2006 .

[5]  Tetsuya Ozaki,et al.  Extraction and mutual separation of rare earths from used polishes by chemical vapor transport , 1999 .

[6]  Bert Bras,et al.  Rare earth metal recycling , 2011, Proceedings of the 2011 IEEE International Symposium on Sustainable Systems and Technology.

[7]  Philippe Guillot,et al.  Re-processing CRT phosphors for mercury-free applications , 2009 .

[8]  Toyohisa Fujita,et al.  Separation of red (Y2O3:Eu3+), blue (BaMgAl10O17:Eu2+) and green (CeMgAl10O17:Tb3) rare earth phosphors by liquid/liquid extraction , 2009 .

[9]  Asaf Pekdeger,et al.  Positive gadolinium anomaly in surface water and ground water of the urban area Berlin, Germany , 2005 .

[10]  T. Ozaki,et al.  Recovery of Rare Earths from Used Polishes by Chemical Vapor Transport Process , 1999 .

[11]  Junmin Nan,et al.  Recovery of metal values from a mixture of spent lithium-ion batteries and nickel-metal hydride batteries , 2006 .

[12]  A. Terziev,et al.  REGENERATION OF WASTE RARE EARTH OXIDES BASED POLISHING MATERIALS , 1996 .

[13]  P. Dulski,et al.  Anthropogenic origin of positive gadolinium anomalies in river waters , 1996 .

[14]  Koen Binnemans,et al.  An environmentally friendlier approach to hydrometallurgy: highly selective separation of cobalt from nickel by solvent extraction with undiluted phosphonium ionic liquids , 2012 .

[15]  Hironori Sato,et al.  Extraction of Sm from Sm–Fe alloys by the glass slag method , 2005 .

[16]  Steven Van Passel,et al.  Enhanced Landfill Mining in view of multiple resource recovery: a critical review , 2013 .

[17]  Jun Sadaki,et al.  Separation of Rare Earth Fluorescent Powders by Two-Liquid Flotation using Organic Solvents , 2008, Japanese Journal of Applied Physics.

[18]  Hironori Sato,et al.  The extraction of Nd from waste Nd-Fe-B alloys by the glass slag method , 2003 .

[19]  Andrew Bradshaw,et al.  The use of hydrogen to separate and recycle NdFeB magnets from electronic waste , 2014 .

[20]  Robert V. Horrigan,et al.  Rare Earth Polishing Compounds , 1981 .

[21]  C. C. Windmöller,et al.  Mercury speciation in fluorescent lamps by thermal release analysis. , 2003, Waste management.

[22]  Masahiro Masuda,et al.  Microwave absorption properties of the nano-composite powders recovered from Nd–Fe–B bonded magnet scraps , 2006 .

[23]  Masahiro Masuda,et al.  Recycling of rare earth sintered magnets as isotropic bonded magnets by melt-spinning , 2004 .

[24]  David Pennington,et al.  Recent developments in Life Cycle Assessment. , 2009, Journal of environmental management.

[25]  Keith Scott,et al.  Recycling of nickel–metal hydride batteries. I: Dissolution and solvent extraction of metals , 2004 .

[26]  D W Pennington,et al.  Life cycle assessment: Part 1: Framework, goal and scope definition, inventory analysis, and applications , 2004 .

[27]  K. Koyama,et al.  Recycling of Rare Earths from Scrap , 2013 .

[28]  Tetsuya Uda,et al.  Recovery of rare earths from magnet sludge by FeCl2 , 2002 .

[29]  Hideaki Itoh,et al.  Consolidation recovery of rare/hazardous elements from polluted water by the hydrothermal mineralization process , 2010 .

[30]  Antonio Gallardo,et al.  Determination of mercury distribution inside spent compact fluorescent lamps by atomic absorption spectrometry. , 2012, Waste management.

[31]  I. R. Harris,et al.  Multiple recycling of NdFeB-type sintered magnets , 2009 .

[32]  Xu Tao,et al.  Formation Cause,Composition Analysis and Comprehensive Utilization of Rare Earth Solid Wastes , 2010 .

[33]  Koen Binnemans,et al.  Lanthanides and actinides in ionic liquids. , 2007, Chemical reviews.

[34]  L. Chumbley,et al.  Liquid metal extraction of Nd from NdFeB magnet scrap , 1999 .

[35]  Masahiro Itoh,et al.  Novel rare earth recovery process on Nd–Fe–B magnet scrap by selective chlorination using NH4Cl , 2009 .

[36]  Nourreddine Menad,et al.  Cathode ray tube recycling , 1999 .

[37]  P. Falconnet The economics of rare earths , 1985 .

[38]  Hongmin Cui,et al.  Recovery of rare earth elements from simulated fluorescent powder using bifunctional ionic liquid extractants (Bif‐ILEs) , 2012 .

[39]  Ryosuke Shimizu,et al.  Supercritical fluid extraction of rare earth elements from luminescent material in waste fluorescent lamps , 2005 .

[40]  P. Lei,et al.  Rare earth extraction and separation from mixed bastnaesite-monazite concentrate by stepwise carbochlorination-chemical vapor transport , 2002 .

[41]  Nobuhiro Nagano,et al.  Separation and Recovery of Rare Earth Elements from Phosphor Sludge in Processing Plant of Waste Fluorescent Lamp by Pneumatic Classification and Sulfuric Acidic Leaching. , 2001 .

[42]  M. D. Dudley Phosphors for cathode-ray tubes in industrial and low scanning speed display systems , 1959 .

[43]  Toru H. Okabe,et al.  Recovery of neodymium from a mixture of magnet scrap and other scrap , 2006 .

[44]  Recovery of rare earth metals from waste material by leaching in non-oxidizing acid and by precipitating using sulphates , .

[45]  V. D. Hildenbrand,et al.  Reduction of Mercury Loss in Fluorescent Lamps Coated with Thin Metal-Oxide Films , 2003 .

[46]  Diran Apelian,et al.  CR3: Cornerstone to the sustainable inorganic materials management (SIM2) research program at K.U.Leuven , 2011 .

[47]  Richard Roth,et al.  Evaluating rare earth element availability: a case with revolutionary demand from clean technologies. , 2012, Environmental science & technology.

[48]  J. J. Croat,et al.  High‐energy product Nd‐Fe‐B permanent magnets , 1984 .

[49]  I. R. Harris,et al.  Possible methods of recycling NdFeB-type sintered magnets using the HD/degassing process , 2008 .

[50]  Alain Rollat,et al.  Process for the recovery of elements of the rare earths from a solid mixture containing a halophosphate and a compound of one or more elements of the rare earths , 2010 .

[51]  Shengming Xu,et al.  Recovery of Ni, Co and rare earths from spent Ni–metal hydride batteries and preparation of spherical Ni(OH)2 , 2009 .

[52]  T. Graedel,et al.  Global in-use stocks of the rare Earth elements: a first estimate. , 2011, Environmental science & technology.

[53]  L. J. Swartzendruber,et al.  The Fe−Mg (Iron-Magnesium) system , 1985 .

[54]  Ken-ichi Machida,et al.  Vapor Phase Extraction and Mutual Separation of Rare Earths from Monazite Using Chemical Vapor Transport Mediated by Vapor Complexes , 1994 .

[55]  F. Ferella,et al.  Treatment of exhaust fluorescent lamps to recover yttrium: experimental and process analyses. , 2011, Waste management.

[56]  Masahiro Itoh,et al.  Extraction of Rare Earth Elements from Nd–Fe–B Magnet Scraps by NH4Cl , 2008 .

[57]  Hideaki Itoh,et al.  Resource Recovery From WastewaterContaining Hazardous OxoanionsBy Hydrothermal Mineralization , 2006 .

[58]  A. P. Bayanov,et al.  DISTRIBUTION OF CERTAIN RARE EARTH ELEMENTS BETWEEN TWO MELTED METALS , 1964 .

[59]  Tetsuji Saito,et al.  Extraction of Tb from Tb–Fe alloys by the glass slag method , 2004 .

[60]  T. Jüstel,et al.  New Developments in the Field of Luminescent Materials for Lighting and Displays. , 1998, Angewandte Chemie.

[61]  Masahiro Itoh,et al.  Effective recycling for Nd-Fe-B sintered magnet scraps , 2006 .

[62]  Loris Pietrelli,et al.  Rare earths recovery from NiMH spent batteries , 2002 .

[63]  Akitsugu Okuwaki,et al.  Recycle of Ceria-Based Glass Polishing Powder Using NaOH Solution. , 2000 .

[64]  He Han-wei,et al.  Recycling rare earth from spent FCC catalyst using P507 (HEH/EHP) as extractant , 2011 .

[65]  Katsutoshi Inoue,et al.  Recovery of metal values from spent nickel–metal hydride rechargeable batteries , 1999 .

[66]  P. Nance,et al.  Human health risks from mercury exposure from broken compact fluorescent lamps (CFLs). , 2012, Regulatory toxicology and pharmacology : RTP.

[67]  Masami Tsunekawa,et al.  Feasibility of an efficient recovery of rare earth-activated phosphors from waste fluorescent lamps through dense-medium centrifugation , 2005 .

[68]  T. Graedel,et al.  Challenges in Metal Recycling , 2012, Science.

[69]  Li Jin,et al.  Environmental Release of Mercury from Broken Compact Fluorescent Lamps , 2011 .

[70]  V. Popov,et al.  Waste Management And the Environment III , 2006 .

[71]  Junmin Nan,et al.  Dismantling, Recovery, and Reuse of Spent Nickel–Metal Hydride Batteries , 2006 .

[72]  E. G. Thaler,et al.  Measurement of Mercury Bound in the Glass Envelope during Operation of Fluorescent Lamps , 1995 .

[73]  Ai Lin Chun Nanoparticle toxicity: Part of the solution , 2007 .

[74]  P. Brunner Urban Mining A Contribution to Reindustrializing the City , 2011 .

[75]  T. Graedel,et al.  Uncovering the Global Life Cycles of the Rare Earth Elements , 2011, Scientific reports.

[76]  J. Allwood,et al.  What Do We Know About Metal Recycling Rates? , 2011 .

[77]  Jurg Keller,et al.  Removal of magnetic resonance imaging contrast agents through advanced water treatment plants. , 2010, Water science and technology : a journal of the International Association on Water Pollution Research.

[78]  Christina H. Chen,et al.  Magnetic Materials and Devices for the 21st Century: Stronger, Lighter, and More Energy Efficient , 2011, Advanced materials.

[79]  Toyohisa Fujita,et al.  A hydrometallurgical process for extraction of lanthanum, yttrium and gadolinium from spent optical glass , 2005 .

[80]  Ungsoo Kim,et al.  Recovery of cerium from glass polishing slurry , 2011 .

[81]  Jianzhuang Jiang,et al.  Separation and recovery of rare earths via a dry chemical vapour transport based on halide gaseous complexes , 1997 .

[82]  Katsutoshi Ono,et al.  Recycling of rare earth magnet scraps: Part I Carbon removal by high temperature oxidation : Special issue on recycling and high performance waste processing , 2001 .

[83]  J. Lyman,et al.  Hydrometallurgical treatment of nickel-metal hydride battery electrodes , 1995 .

[84]  Atsushi Shibayama,et al.  RECOVERY OF RARE EARTHS FROM THE SPENT OPTICAL GLASS BY HYDROMETALLURGICAL PROCESS , 2004 .

[85]  H. Okamoto,et al.  Mg-Nd (Magnesium-Neodymium) , 1991 .

[86]  Motohide Matsuda,et al.  Recovery of rare metal compounds from nickel-metal hydride battery waste and their application to CH4 dry reforming catalyst. , 2009, Journal of hazardous materials.

[87]  Arvid Ödegaard-Jensen,et al.  Using Cyanex 923 for selective extraction in a high concentration chloride medium on nickel metal hydride battery waste , 2012 .

[88]  Katsutoshi Ono,et al.  Recycling of rare earth magnet scraps. Part III. Carbon removal from Nd magnet grinding sludge under vacuum heating , 2002 .

[89]  T. Dang,et al.  Applications of surface analytical techniques for study of the interactions between mercury and fluorescent lamp materials , 2002, Analytical and bioanalytical chemistry.

[90]  D. Fontana,et al.  Characterization and leaching of NiCd and NiMH spent batteries for the recovery of metals. , 2005, Waste management.

[91]  Matthias Kaindl,et al.  Recycling von Seltene Erden aus Nickel-Metallhydrid-Akkumulatoren unter besonderer Berücksichtigung von Säurerückgewinnung , 2012, BHM Berg- und Hüttenmännische Monatshefte.

[92]  M. Goto,et al.  Selective recovery of dysprosium and neodymium ions by a supported liquid membrane based on ionic liquids , 2011 .

[93]  Tobias Müller,et al.  Development of a recycling process for nickel-metal hydride batteries , 2006 .

[94]  M. Buchert,et al.  Recycling critical raw materials from waste electronic equipment , 2012 .

[95]  Tetsuya Ozaki,et al.  Extraction and mutual separation of rare earths from concentrates and crude oxides using chemical vapor transport , 1996 .

[96]  Junya Kano,et al.  Estimation of Extraction Rate of Yttrium from Fluorescent Powder by Ball Milling. , 2001 .

[97]  Fukuda Tadashi,et al.  Recycling of rare earth magnet scraps: Carbon and oxygen removal from Nd magnet scraps , 2006 .

[98]  Ken-ichi Machida,et al.  Recovery of rare metals from scrap of rare earth intermetallic material by chemical vapour transport , 1995 .

[99]  Akitsugu Okuwaki,et al.  Study for Recycling of Ceria-Based Glass Polishing Powder , 2000 .

[100]  Guangjun Mei,et al.  Separation of red (Y2O3: Eu3+), blue (Sr, Ca, Ba)10(PO4)6Cl2: Eu2+ and green (LaPO4: Tb3+, Ce3+) rare earth phosphors by liquid/liquid extraction , 2009 .

[101]  Masahiro Itoh,et al.  Extraction and recovery characteristics of Fe element from Nd-Fe-B sintered magnet powder scrap by carbonylation , 2008 .

[102]  K.H.J. Buschow Trends in Rare Earth Permanent Magnets , 1995 .

[103]  M. Goto,et al.  Recent Advances in Extraction and Separation of Rare-Earth Metals Using Ionic Liquids , 2011 .

[104]  Hironori Sato,et al.  Extraction of Sm from Sm-Fe-N magnets by the glass slag method , 2005 .

[105]  Kyeong Woo Chung ChulJoo Kim,et al.  Selective leaching of rare earth elements from NdFeB powders via alkaline treatment and thermal oxidation , 2015 .

[106]  Ken-ichi Machida,et al.  Rare Earth Separation Using Chemical Vapor Transport with LnCl3-AlCl3 Gas Phase Complexes. , 1991 .

[107]  Katsutoshi Inoue,et al.  Hydrometallurgical process for recovery of metal values from spent nickel-metal hydride secondary batteries , 1998 .

[108]  Lauri Niinistö,et al.  Industrial applications of the rare earths, an overview , 1987 .

[109]  T. A. Dang,et al.  Identification of Mercury Reaction Sites in Fluorescent Lamps , 1999 .

[110]  Marcelo Borges Mansur,et al.  Hydrometallurgical separation of rare earth elements, cobalt and nickel from spent nickel–metal–hydride batteries , 2010 .

[111]  Pornpote Piumsomboon,et al.  LCA of spent fluorescent lamps in Thailand at various rates of recycling , 2008 .

[112]  K. Scott,et al.  RECYCLING | Nickel–Metal Hydride Batteries , 2009 .

[113]  C. Ronda,et al.  Phosphors for Lamps and Displays: An Applicational View , 1995 .

[114]  M. Rabah,et al.  Recyclables recovery of europium and yttrium metals and some salts from spent fluorescent lamps. , 2008, Waste management.

[115]  I. R. Harris,et al.  Anisotropic powder from sintered NdFeB magnets by the HDDR processing route , 2012 .

[116]  A. Otsuki,et al.  Separation of a mixture of rare earth fluorescent powders by two-liquid flotation using polar and non-polar organic solvents for recycling , 2007, 2007 Digest of papers Microprocesses and Nanotechnology.

[117]  Timothy W. Ellis,et al.  Methods and opportunities in the recycling of rare earth based materials , 1994 .

[118]  Qin Yu-fan,et al.  Recovery of Rare Earths from Waste Catalyst , 2014 .

[119]  E. G. Thaler,et al.  Mercury‐Glass Interactions in Fluorescent Lamps , 1995 .

[120]  Fumio Saito,et al.  Sonochemical Recovery of Metals from Recording Media , 2002 .

[121]  Patrick R. Taylor,et al.  Survey of recycled rare earths metallurgical processing , 2013 .

[122]  Toru H. Okabe,et al.  Phase equilibrium of the system Ag–Fe–Nd, and Nd extraction from magnet scraps using molten silver , 2004 .

[123]  T. Graedel,et al.  Global Rare Earth In‐Use Stocks in NdFeB Permanent Magnets , 2011 .

[124]  Masami Tsunekawa,et al.  Floatability of rare earth phosphors from waste fluorescent lamps , 2005 .

[125]  François Grosse,et al.  Is recycling “part of the solution”? The role of recycling in an expanding society and a world of finite resources , 2010 .

[126]  Hideaki Itoh,et al.  A Novel Recovery Method for Treating Wastewater Containing Fluoride and Fluoroboric Acid , 2006 .

[127]  M. Humphries Rare Earth Elements: The Global Supply Chain [September 30, 2010] , 2010 .

[128]  Hideaki Itoh,et al.  Arsenic Recovery from Water Containing Arsenite Ions by Hydrothermal Mineralization , 2006 .

[129]  Hironori Sato,et al.  Recovery of rare earths from sludges containing rare-earth elements , 2006 .

[130]  Michael Bredol,et al.  Leuchtstoffe für Kathodenstrahlröhren , 1994 .

[131]  Toru H. Okabe,et al.  Phase Equilibria of the System Fe—Mg—Nd at 1076 K. , 2005 .

[132]  아그니에스츠카 오즈타레비츠-카스프르작,et al.  Method for recovery of rare earths from fluorescent lamps , 2007 .

[133]  I. R. Harris,et al.  Hydrogen Decrepitation and Recycling of NdFeB-type Sintered Magnets , 2006 .

[134]  艾伯特·A·维尔海利希 Methods of recovering rare earth elements , 2012 .

[135]  MasahiroItoh,et al.  Recycle for Sludge Scrap of Nd-Fe-B Sintered Magnet as Isotropic Bonded Magnet , 2004 .

[136]  Akitsugu Okuwaki,et al.  Study for Recycling of Ceria-Based Glass Polishing Powder II−Recovery of Hydroxysodalite from the Alkali Waste Solution Containing SiO2 and Al2O3 , 2000 .

[137]  Katsutoshi Ono,et al.  Recycling of rare earth magnet scraps: Part II Oxygen removal by calcium : Special issue on recycling and high performance waste processing , 2001 .

[138]  Hideaki Itoh,et al.  In Situ Solid/Liquid Separation Effect for High-Yield Recovery of Boron and Fluorine from Aqueous Media Containing Borate or Fluoroborate Ions , 2007 .

[139]  Guocai Zhu,et al.  Separation and recovery of RE and Mn from MN rare earth mud in China , 2000 .

[140]  C. Hagelüken,et al.  Securing the supply for tomorrow : Precious metals recycling from automotive catalysts , 2001 .

[141]  Toru H. Okabe,et al.  Direct Extraction and Recovery of Neodymium Metal from Magnet Scrap , 2003 .

[142]  Xiahui Wang,et al.  Notice of RetractionRecovery of Rare Earths from Spent Fluorescent Lamps , 2011, 2011 5th International Conference on Bioinformatics and Biomedical Engineering.

[143]  V. D. Hildenbrand,et al.  Interactions of thin oxide films with a low-pressure mercury discharge , 2000 .

[144]  Ken-ichi Machida,et al.  Rare earth separation using chemical vapor transport with LnCl3AlCl3 gas phase complexes , 1991 .

[145]  Denise Crocce Romano Espinosa,et al.  Metal separation from mixed types of batteries using selective precipitation and liquid-liquid extraction techniques. , 2011, Waste management.

[146]  N.Yu. Pribyl'skii,et al.  Phase equilibria of the Gd-Se system , 1982 .

[147]  J. K. Park,et al.  Characterization and recovery of mercury from spent fluorescent lamps. , 2005, Waste management.

[148]  Hironori Sato,et al.  The Extraction of Sm from Sm-Co alloys by the Glass Slag Method , 2003 .

[149]  G Finnveden,et al.  Life cycle assessment part 2: current impact assessment practice. , 2004, Environment international.

[150]  Michael Mccoy A MARKET GROWS, BLOCK BY BLOCK , 2011 .