Skip to main content
Log in

Evaluation of Baking Process for Rare-Earth Recovery from Discarded Tube Lights Phosphor

  • Published:
Mining, Metallurgy & Exploration Aims and scope Submit manuscript

Abstract

The current study examines the extraction of rare-earth elements from trichromatic phosphor of discarded tube lights via baking processes. The Y2O3:Eu3+ (YOX) and BaMgAl10O17:Eu2+ (BAM) phases completely decomposed during acid and alkali baking with > 90% Eu and Y extraction. Prior, selective acid leaching of the YOX phase enhanced the acid baking process at a lower temperature (< 230 ℃). Feed acid baking showed a maximum 87% Tb, 36% La, and 17% Ce extraction at 500 °C, 0.5 h, 1 ml/g H2SO4, and alkali baking yielded 16.1% Tb, 86% La, and 73% Ce at 300 ℃, 0.5 h, 50 wt.% NaOH. The acid baking of the acid-leached phosphor yielded 72% Tb, 95% La, 63% Ce, ~ 95% Y, and Eu extraction at 300 °C, 0.5 h, 1.05 mL/g H2SO4. Lower Tb extraction during the acid baking of acid-leached phosphor can be attributed to the formation of Ba3Tb(PO4)3 and BaTbO3 phases. Insoluble Si3Tb5 phase formation and partial decomposition of CeMgAl11O19:Tb3+ (CMAT) phase in the alkali baking route leads to lower Tb extraction. The acid baking process is suitable for extracting Tb, Eu, and Y, whereas the alkali baking process is suitable for La and Ce. The thermal analysis of phosphor and flux interaction depicts that alkali baking is less energy-intensive than acid baking. In comparison, the one-step acid baking process and the two-step alkali baking process yielded desirable extraction results (87% Tb, total RE (rare earth) 78.5% and 50.4% Tb, total RE 59.3%). The product yield in the acid and alkali baking route of feed, acid-leach phosphor is 36%, 29%, and 39%, 28.2%, respectively, with ~ 98% mixed rare-earth oxide purity.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10
Fig. 11
Fig. 12

Similar content being viewed by others

References

  1. Anand A, Singh R (2021) Synthesis of Rare Earth Compounds from Phosphor Coating of Spent Fluorescent Lamps. Sep Purif Review 50(1):96–112

    Article  MathSciNet  Google Scholar 

  2. Innocenzi V (2018) Treatment of spent fluorescent lamps, cathode-ray tubes, and spent catalysts by hydrometallurgical procedures, WEEE 139–160. Woodhead Publishing

    Google Scholar 

  3. Zhang J, Zhang Z, Tang Z, Lin Y (2001) Mn2+ luminescence in (Ce, Tb) MgAl11O19 phosphor. Mater Chem Phys 72(1):81–84

    Article  Google Scholar 

  4. Binnemans K, Jones P (2014) Perspectives for the recovery of rare earths from end-of-life fluorescent lamps. J Rare Earths 32(3):195–200

    Article  Google Scholar 

  5. Belardi G, Ippolito N, Piga L, Serracino M (2014) Investigation on the status of rare earth elements contained in the powder of spent fluorescent lamps. Thermochim Acta 591:22–30

    Article  Google Scholar 

  6. Dhawan N, Tanvar H (2022) A critical review of end-of-life fluorescent lamps recycling for recovery of rare earth values. Sustain Mater Technol 32:e00401. https://doi.org/10.1016/j.susmat.2022.e00401

  7. Hirajima T, Sasaki K, Bissombolo A, Hirai H, Hamada M, Tsunekawa M (2005) Feasibility of an efficient recovery of rare earth-activated phosphors from waste fluorescent lamps through dense-medium centrifugation. Sep Purif Technol 44(3):197–204

    Article  Google Scholar 

  8. Mei G, Rao P, Matsuda M, Fujita T (2009) Separation of red (Y2O3: Eu3+), blue (BaMgAl10O17: Eu2+) and green (CeMgAl10O17: Tb3+) rare earth phosphors by liquid/liquid extraction. J Wuhan Univ Technol Mater Sci Ed. 24(4): 603–607

  9. Otsuki A, Dodbiba G, Shibayama A, Sadaki J, Mei G, Fujita T (2008) Separation of rare earth fluorescent powders by two-liquid flotation using organic solvents. Jpn J Appl Phys 47:5093

    Article  Google Scholar 

  10. Mei G, Rao P, Mitsuaki M, Toyohisa F (2009) 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. J Wuhan Univ Technol Mater Sci Ed. 24(3):418–423.

  11. Yamashita M, Akai T, Murakami M, Oki T (2018) Recovery of LaPO4: Ce3+, Tb3+ from waste phosphors using high-gradient magnetic separation. Waste Manage 79:164

    Article  Google Scholar 

  12. Eduafo P, Mishra B (2018) Leaching kinetics of yttrium and europium oxides from waste phosphor powder. J Sustain Metall 4(4):437–442

    Article  Google Scholar 

  13. Tunsu C, Lapp J, Ekberg C, Retegan T (2016) Selective separation of yttrium and europium using Cyanex 572 for applications in fluorescent lamp waste processing. Hydrometallurgy 166:98–106

  14. Tan Q, Deng C, Li J (2017) Enhanced recovery of rare earth elements from waste phosphors by mechanical activation. J Clean Prod 142:2187–2191

    Article  Google Scholar 

  15. Van Loy S, Binnemans K, Van Gerven T (2017) Recycling of rare earths from lamp phosphor waste: Enhanced dissolution of LaPO4:Ce3+, Tb3+ by mechanical activation. J Clean Prod 156:226–234

    Article  Google Scholar 

  16. United States Geological Survey Website (USGS) (2020) Commodity Statistics and Information. Available http://minerals.usgs.gov/minerals/pubs/commodity/ [Accessed 10 Feb 2021]

  17. Binnemans K, Jones P, Blanpain B, Van Gerven T, Yang Y, Walton A, Buchert M (2013) Recycling of rare earths: a critical review. J Clean Prod 51:1–22

    Article  Google Scholar 

  18. Tunsu C, Ekberg C, Retegan RT (2014) Characterization and leaching of real fluorescent lamp waste for the recovery of rare earth metals and mercury. Hydrometallurgy 144–145:91–98

  19. De Carolis R, Fontana D, Pietrantonio M, Pucciarmati S, Torelli G (2015) A Hydrometallurgical Process for Recovering Rare Earths and Metals from Spent Fluorescent Lamps. Environ Eng Manag J 14(7):1603–1609

    Article  Google Scholar 

  20. Innocenzi V, Ippolito N, De Michelis I, Medici F, Vegliò F (2016) A hydrometallurgical process for the recovery of terbium from fluorescent lamps: experimental design, optimization of acid leaching process and process analysis. J Environ Manage 184:552–559

    Article  Google Scholar 

  21. Miskufova A, Kochmanova A, Havlik T, Horvathova H, Kuruc P (2018) Leaching of yttrium, europium and accompanying elements from phosphor coatings. Hydrometallurgy 176:216–228

  22. Burgess WA, Keller MJ, Lekse JW, Howard BH, Roth EA, Granite EJ (2018) Effect of pre-reaction ball milling on kinetics of lanthanum phosphate roasting with sodium carbonate. Ind Eng Chem Res 57(18):6088–6096

    Article  Google Scholar 

  23. Song G, Yuan W, Zhu X, Wang X, Zhang C, Li J, Bai J, Wang J (2017) Improvement in rare earth element recovery from waste trichromatic phosphors by mechanical activation. J Clean Prod 151:361–370

    Article  Google Scholar 

  24. Liang Y, Liu Y, Lin R, Guo D, Liao C (2016) Leaching of rare earth elements from waste lamp phosphor mixtures by reduced alkali fusion followed by acid leaching. Hydrometallurgy 163:99–103

  25. Zhang S, Liu H, Pan D, Tian J, Liu Y, Volinsky A (2015) Complete recovery of Eu from BaMgAl10 O17: Eu2+ by alkaline fusion and its mechanism. RSC Adv 5(2):1113–2111

    Article  Google Scholar 

  26. Liu H, Zhang S, Pan D, Liu Y, Liu B, Tian J, Volinsky A (2015) Mechanism of CeMgAl11O19: Tb3+ alkaline fusion with sodium hydroxide. Rare Met 34(3):189–194

    Article  Google Scholar 

  27. Ippolito N, Innocenzi V, De Michelis I, Medici F, Vegliò F (2017) Rare earth elements recovery from fluorescent lamps: A new thermal pretreatment to improve the efficiency of the hydrometallurgical process. J Clean Prod 153:287–298

    Article  Google Scholar 

  28. Ippolito N, Ferella F, Innocenzi V, Trapasso F, Passeri D, Belardi G, Vegliò F (2021) Effect of mechanical activation on terbium dissolution from waste fluorescent powders. Miner Eng 167:106906

    Article  Google Scholar 

  29. Braconnier J, Rollat A (2010) Process for recovery of rare earths starting from a solid mixture containing a halophosphate and a compound of one or more rare earths. Patent WO2010118967A1 (Rhodia Operations, France)

  30. Liu H, Li S, Wang B, Wang K, Wu R, Ekberg C, Volinsky A (2019) Multiscale recycling rare earth elements from real waste trichromatic phosphors containing glass. J Clean Prod 238:117998

    Article  Google Scholar 

  31. Yurramendi L, Gijsemans L, Forte F, Aldana J, del Río C, Binnemans K (2019) Enhancing rare-earth recovery from lamp phosphor waste. Hydrometallurgy 187:38–44

    Article  Google Scholar 

  32. Yu M, Mei G, Chen X (2018) Recovering rare earths and aluminum from waste BaMgAl10O17: Eu2+ and CeMgAl11O19: Tb3+ phosphors using NaOH sub-molten salt method. Miner Eng 117:1–7

    Article  Google Scholar 

  33. Liu H, Zhang S, Pan D, Tian J, Yang M, Wu M, Volinsky AA (2014) Rare earth elements recycling from waste phosphor by dual hydrochloric acid dissolution. J Hazard Mater 272:96–101

    Article  Google Scholar 

  34. Innocenzi V, De Michelis I, Ferella F, Vegliò F (2017) Secondary yttrium from spent fluorescent lamps: recovery by leaching and solvent extraction. Int J Miner Process 168:87–94

    Article  Google Scholar 

  35. Innocenzi V, Ippolito N, Pietrelli L, Centofanti M, Piga L, Vegliò F (2018) Application of solvent extraction operation to recover rare earths from fluorescent lamps. J Clean Prod 172:2840–2852

    Article  Google Scholar 

  36. da Siva L, Nascimento M, de Oliveira E, de Queiroz A, Fernandes M, de Castro J (2020) Evaluation of the diffusional coefficient in the acid baking process using microwave energy to reduce phosphorus content in iron ore particles. Min Eng 157:106541

    Article  Google Scholar 

  37. Kul M, Topkaya Y, Karakaya I (2008) Rare earth double sulfates from pre-concentrated bastnasite. Hydrometallurgy 93(3–4):129–135

  38. Teixeira L, Silva R, Majuste D, Ciminelli V (2020) Stability of lanthanum in sulfate and phosphate systems and implications for selective rare earths extraction. Min Eng 155:106440

    Article  Google Scholar 

  39. Demol J, Ho E, Senanayake G (2018) Sulfuric acid baking and leaching of rare earth elements, thorium and phosphate from a monazite concentrate: Effect of bake temperature from 200 to 800 °C. Hydrometallurgy 179:254–267

  40. Zou D, Li H, Deng Y, Chen J, Bai Y (2021) Recovery of lanthanum and cerium from rare earth polishing powder wastes utilizing acid baking-water leaching-precipitation process. Sep Purific Technol 261:118244

    Article  Google Scholar 

  41. Shukla N, Dhawan N (2020) Investigation of Different Processing Routes for Rare Earth Extraction from Discarded Tubular Lights. J Sustain Metall 6(2):269–280

    Article  Google Scholar 

  42. Shukla N, Dhawan N (2020) Rapid microwave processing of discarded tubular lights for extraction of rare earth values. Pro Saf Environ Protect 142:238–249

    Article  Google Scholar 

  43. Shukla N, Tanvar H, Dhawan N (2020) Evaluation of alkali processing for the recycling of rare earth values from spent fluorescent lamps. Physicochem Probl Miner Process 56(4):710–722

    Google Scholar 

  44. Shukla N, Agrawal S, Dhawan N (2021) Microwave acid baking process for recovery of rare-earth concentrate from phosphor of end-of-life fluorescent lamps. J Clean Prod 307:127235

    Article  Google Scholar 

  45. Shukla N, Dhawan N (2021) Processing End-of-Life Tube Lights for Recovery of Rare Earth Oxides. JOM 73(4):1090–1102

    Article  Google Scholar 

  46. Borra C, Mermans J, Blanpain B, Pontikes Y, Binnemans K, Van Gerven T (2016) Selective recovery of rare earths from bauxite residue by combination of sulfation, roasting and leaching. Min Eng 92:151–159

    Article  Google Scholar 

  47. Liu Y, Zhang S, Liu H, Liu B, Volinsky AA, Chang C (2015) Free oxoanion theory for BaMgAl10O17: Eu2+ structure decomposition during alkaline fusion process. RSC Adv 5(62):50105–50112

    Article  Google Scholar 

  48. Kumar U, Gaikwad V, Sahajwalla V (2018) Transformation of waste toner to iron using E-waste plastics as a carbon resource. J Clean Prod 192:244–251

    Article  Google Scholar 

  49. Trinh H, Lee J, Kim S, Kim J (2020) Recovery of Cerium from Spent Autocatalyst by Sulfatizing–Leaching–Precipitation Process. ACS Sust Chem Eng 8(41):15630–15639

    Article  Google Scholar 

  50. Paulenova A, Creager S, Navratil J, Wei Y (2002) Redox potentials and kinetics of the Ce3+/Ce4+ redox reaction and solubility of cerium sulfates in sulfuric acid solutions. J Power Sources 109:431–438

    Article  Google Scholar 

  51. Pelczarska A, Radomińska E, Znamierowska T (2020) Eulytite-type solid solution in the LaPO4–Ba3(PO4)2 system. J Alloys Compd 822:153550

    Article  Google Scholar 

  52. Kunzler J, Giauque W (1952) Aqueous Sulfuric Acid. Heat Capacity. Partial Specific Heat Content of Water at 25 and-20. J Am Chem Soc 74(14):3472–3476

    Article  Google Scholar 

  53. Thiyagarajan T, Sreekumar K, Selvan V, Ramachandran K, Ananthapadmanabhan P (2010) Simulation studies to optimize the process of plasma spray deposition of yttrium oxide. In J Phys Conf Ser 208(1):012116

Download references

Acknowledgements

The authors acknowledge the funding received from the Indian Insitute of Technology, Roorkee (Faculty Initiation Grant; FIG-100714), and Shrey Agrawal for valuable discussions.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Nikhil Dhawan.

Ethics declarations

Conflict of Interest

The authors declare no competing interests.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary Information

Below is the link to the electronic supplementary material.

Supplementary file1 (DOCX 153 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Shukla, N., Dhawan, N. Evaluation of Baking Process for Rare-Earth Recovery from Discarded Tube Lights Phosphor. Mining, Metallurgy & Exploration 39, 1571–1586 (2022). https://doi.org/10.1007/s42461-022-00598-w

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s42461-022-00598-w

Keywords

Navigation