Skip to main content
Log in

A continuous high-efficient demetallization strategy for used lubricating oils resource utilization

  • ORIGINAL ARTICLE
  • Published:
Journal of Material Cycles and Waste Management Aims and scope Submit manuscript

Abstract

Resource utilization of used lubricating oils (ULO) has attracted a great deal of attention over the last few decades, but remains a huge challenge. Hydrogenation has been used as an environmentally friendly ULO regeneration process. In this research, a novel high-efficient continuous process based on thermal demetallization has been proposed to solve the critical problem that high metal content limits the regeneration hydrogenation process of ULO. Metal removal rate can reach 99.2%. At the same time, a reaction kinetic model of demetallization has been established. The demetallization products which have been rarely identified using experimental methods, have been studied using FT-IR and XPS. Results estimated that the pyrolysis demetallization process is accomplished by the transformation of the additives in ULO into sludge and carbonaceous deposits. To understand the demetallization pathway, a simulation of the carbon deposition process has been carried out using tubing bomb experiment. SEM of the carbon deposit products was consistent with the results obtained for the demetallization residues. Finally, distillation process analysis of the ULO thermal demetallization samples obtained at the highest temperature verified that heating has little effect on the basic properties of lubricant base oil, which further verifies the feasibility of the method.

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

Similar content being viewed by others

Data availability

Due to the nature of this research, participants of this study did not agree for their data to be shared publicly, so supporting data is not available.

References

  1. Santos JCO, Almeida RA, Carvalho MWNC, Lima AEA, Souza AG (2019) Recycling of lubricating oils used in gasoline/alcohol engines. J Therm Anal Calorim 137(4):1463–1470

    Article  Google Scholar 

  2. Lam SS, Liew RK, Jusoh A, Chong CT, Ani FN, Chase HA (2016) Progress in waste oil to sustainable energy, with emphasis on pyrolysis techniques. Renew Sustain Energy Rev 53:741–753. https://doi.org/10.1016/j.rser.2015.09.005

    Article  Google Scholar 

  3. Refining Used Lubricating Oils. CRC Press. Founding Editor is Heinz Heinemann (Berkeley, California), Series Editor is James G. Speight (CD & W, Inc.Laramie, Wyoming). International Standard Book Number-13: 978-1-4665-5150-3 (eBook - PDF).

  4. Wetwatana U, Kim-Lohsoontorn P, Assabumrungrat S, Laosiripojana N (2010) Catalytic steam and autothermal reforming of Used Lubricating Oil (ULO) over Rh- and Ni-based catalysts. Ind Eng Chem Res 49(21):10981–10985

    Article  Google Scholar 

  5. Kamal MA, Naqvi SMD, Khan F (2013) The characterization of indigenous magnesite: a prospective adsorbent for the re-refining of used lubricating oil. Pet Sci Technol 31(22):2348–2356

    Article  Google Scholar 

  6. Kanokkantapong V, Kiatkittipong W, Panyapinyopol B, Wongsuchoto P, Pavasant P (2009) Used lubricating oil management options based on life cycle thinking. Resour Conserv Recycl 53(5):294–299

    Article  Google Scholar 

  7. Guerin TF (2008) Environmental liability and life-cycle management of used lubricating oils. J Hazard Mater 160(2):256–264

    Article  Google Scholar 

  8. Ali Durrani H (2014) Re-refining recovery methods of used lubricating oil. Int J Eng Sci Res Technol 3(3):1216–1220

    Google Scholar 

  9. Izza H, Abdessalam SB, Bouida M, Haddad A (2018) Recycling of used motor oil as an alternative method for production feedstock for the conversion processes. Pet Sci Technol 36(19):1511–1515

    Article  Google Scholar 

  10. Zubaidy EAH, Abouelnasr DM (2010) Fuel recovery from waste oily sludge using solvent extraction. Process Saf Environ Prot 88(5):318–326

    Article  Google Scholar 

  11. Rincón J, Cañizares P, García MT (2007) Regeneration of used lubricant oil by ethane extraction. J Supercrit Fluid 39(3):315–322

    Article  Google Scholar 

  12. Hamawand I, Yusaf T, Rafat S (2013) Recycling of waste engine oils using a new washing agent. Energies 6(2):1023–1049

    Article  Google Scholar 

  13. Rincon J, Cañizares P, García M, Gracia I (2003) Regeneration of used lubricant oil by propane extraction. Ind Eng Chem Res 42:4867–4873

    Article  Google Scholar 

  14. Tur E, Onal-Ulusoy B, Akdogan E, Mutlu M (2012) Surface modification of polyethersulfone membrane to improve its hydrophobic characteristics for waste frying oil filtration: Radio frequency plasma treatment. J Appl Polym Sci 123(6):3402–3411

    Article  Google Scholar 

  15. Dang G (1997) Rerefining of used oils-a review of commercial processes. Tribotest 3:445–457

    Article  Google Scholar 

  16. Wang F, Li ML, Duan PG, Fu J, Lü XY, Xu YP (2016) Co-hydrotreating of used engine oil and the low-boiling fraction of bio-oil blends for the production of liquid fuel. Fuel Process Technol 146:62–69

    Article  Google Scholar 

  17. Sychra V, Lang I, Sebor G (1981) Analysis of petroleum and petroleum products by atomic absorption spectroscopy and related techniques. Prog Anal At Spectrosc 4:341–426

    Google Scholar 

  18. Shang H, Liu Y, Shi JC, Shi Q, Zhang WH (2016) Microwave-assisted nickel and vanadium removal from crude oil. Fuel Process Technol 142:250–257

    Article  Google Scholar 

  19. Kressmann S, Morel F, Harlé V, Kasztelan S (1998) Recent developments in fixed-bed catalytic residue upgrading. Catal Today 43(3):203–215

    Article  Google Scholar 

  20. Lázaro MJ, Moliner R, Domeño C, Nerı́n, C. (2001) Low-cost sorbents for demetalisation of waste oils via pyrolysis. J Anal Appl Pyrolysis 57(1):119–131

    Article  Google Scholar 

  21. Leyva C, Rana MS, Trejo F, Ancheyta J (2009) NiMo supported acidic catalysts for heavy oil hydroprocessing. Catal Today 141(1):168–175

    Article  Google Scholar 

  22. Wen Z, Yang J, Xu X, Gao J (2013) Removal of nickel and vanadium from crude oil by microwave-chemical method. I. Chemical method. Pet Sci Technol 31(9):991–999

    Article  Google Scholar 

  23. Zhang Y, Cui Y, Liu S, Fan L, Zhou N, Peng P, Wang Y, Guo F, Min M, Cheng Y, Liu Y, Lei H, Chen P, Li B, Ruan R (2020) Fast microwave-assisted pyrolysis of wastes for biofuels production - a review. Bioresour Technol 297:122480

    Article  Google Scholar 

  24. Muelas A, Aranda D, Callen MS, Murillo R, Veses A, Asrardel M, Ballester J (2020) Properties and combustion characteristics of bio-oils from catalytic co-pyrolysis of grape seeds, polystyrene, and waste tires. Energy Fuels 34(11):14190–14203

    Article  Google Scholar 

  25. Sainz-Diaz CI, Kelly DR, Avenell CS, Griffiths AG (1997) Pyrolysis of furniture and tire wastes in a flaming pyrolyzer minimizes discharges to the environment. Energy Fuels 11(5):1061–1072

    Article  Google Scholar 

  26. Song C, Eser S, Schobert HH, Hatcher PG (1993) Pyrolytic degradation studies of a coal-derived and a petroleum-derived aviation jet fuel. Energy Fuels 7(2):234–243

    Article  Google Scholar 

  27. Silveira E, Coelho R, Moita Neto J, Moura C, Moura E (2009) Determination of metals in lubricating oils, from public transportation, using the FAAS. Quim Nova 33:1863–1867

    Article  Google Scholar 

  28. Sousa Rios MA, Mazzetto SE (2013) Effect of organophosphate antioxidant on the thermo-oxidative degradation of a mineral oil. J Therm Anal Calorim 111(1):553–559

    Article  Google Scholar 

  29. Guan L, Feng XL, Xiong G, Xie JA (2011) Application of dielectric spectroscopy for engine lubricating oil degradation monitoring. Sens Actuators A 168(1):22–29

    Article  Google Scholar 

  30. Watcharasing S, Kongkowit W, Chavadej S (2009) Motor oil removal from water by continuous froth flotation using extended surfactant: effects of air bubble parameters and surfactant concentration. Sep Purif Technol 70(2):179–189

    Article  Google Scholar 

  31. Santos JCO, Oliveira AD, Silva CC, Silva JDS, Souza AG, Lima LN (2007) Kineticand activation thermodynamic parameters on thermal decomposition of syntheticlubricant oils. J Therm Anal Calorim 87(3):823–829

    Article  Google Scholar 

  32. Santos JCO, Lima LN, Santos IMG, Souza AG (2007) Thermal, spectroscopic and rheological study of mineral base lubricating oils. J Therm Anal Calorim 87(3):639–643

    Article  Google Scholar 

  33. Santos J, Lima L, Souza A (2007) Thermoanalytical and kinetic study of lubricating lithium greases. J Eng Appl Sci 2:718–721

    Google Scholar 

  34. Santos J, Sousa A (2006) Liquid specific heat capacity of motor lubricant oils after thermal degradation. J Eng Appl Sci 1:495–499

    Google Scholar 

  35. Santos JCO, dor Santos IMG, Souza AG, Sobrinho EV, Fernandes VJ, Silva AJN (2004) Thermoanalytical and rheological characterization of automotive mineral lubricants after thermal degradation. Fuel 83(17):2393–2399

    Article  Google Scholar 

  36. Castner DG, Hinds K, Grainger DW (1996) X-ray photoelectron spectroscopy sulfur 2p study of organic thiol and disulfide binding interactions with gold surfaces. Langmuir 12(21):5083–5086

    Article  Google Scholar 

  37. Adham A, Farhad K, Gray M (2007) Kinetic modeling of demetalization reactions of topped athabasca bitumen. Pet Coal 49:41

    Google Scholar 

  38. Behar F, Lorant F, Budzinski H, Desavis E (2002) Thermal stability of alkylaromatics in natural systems: kinetics of thermal decomposition of dodecylbenzene. Energy Fuels 16:831–841

    Article  Google Scholar 

  39. Hunter K, East A (2002) Properties of C-C Bonds in n-Alkanes: Relevance to Cracking Mechanisms. J Phys Chem A 106:1346–1356. https://doi.org/10.1021/jp0129030

    Article  Google Scholar 

  40. Xiao YT, Longo JM, Hieshima GB, Hill RJ (1997) Understanding the kinetics and mechanisms of hydrocarbon thermal cracking: an ab initio approach. Ind Eng Chem Res 36:4033–4040. https://doi.org/10.1021/ie960724c

    Article  Google Scholar 

  41. Cai Z, Zhuang X, Yang X, Huang F, Wang Y, Li Y (2021) Litsea cubeba kernel oil as a promising new medium-chain saturated fatty acid feedstock for biolubricant base oil synthesis. Ind Crops Prod 167:113564

    Article  Google Scholar 

  42. Gan Z, Yao T, Zhang M, Hu J, Liao X, Shen Y (2020) Effect of temperature on the composition of a synthetic hydrocarbon aviation lubricating oil. Materials 13(7):1606

    Article  Google Scholar 

  43. Yao T, Zhang N, Hu J, Liao X, Shen Y, Gan Z (2020) Effect of temperature on the chemical composition and physicochemical properties of diester aviation lubrication oil. Int J Chem Eng. https://doi.org/10.1155/2020/8829206

    Article  Google Scholar 

  44. Abou El Naga HH, Salem AEM (1986) Testing thermal stabilities of base oils and their additives via high-temperature infrared spectroscopy. J Therm Anal 31(4):747–759

    Article  Google Scholar 

  45. Zhang Y, Jiang H, Wang K, Wang H, Wang C (2020) Green flotation of polyethylene terephthalate and polyvinyl chloride assisted by surface modification of selective CaCO3 coating. J Clean Prod 242:118441

    Article  Google Scholar 

  46. Jeon KW, Seo DK (2014) Concomitant thionation and reduction of graphene oxide through solid/gas metathetical sulfidation reactions at high temperatures. Phosphorus Sulfur Silicon Relat Elem 189(6):721–737

    Article  Google Scholar 

  47. Crispin X, Marciniak S, Osikowicz W, Zotti G, van der Gon AWD, Louwet F, Fahlman M, Groenendaal L, De Schryver F, Salaneck WR (2003) Conductivity, morphology, interfacial chemistry, and stability of poly(3,4-ethylene dioxythiophene)–poly(styrene sulfonate): a photoelectron spectroscopy study. J Polym Sci, Part B: Polym Phys 41(21):2561–2583

    Article  Google Scholar 

  48. Hutchison JE, Postlethwaite TA, Murray RW (1993) Molecular films of thiol-derivatized tetraphenylporphyrins on gold: film formation and electrocatalytic dioxygen reduction. Langmuir 9(11):3277–3283

    Article  Google Scholar 

  49. Crobu M, Rossi A, Spencer ND (2012) Effect of chain-length and countersurface on the tribochemistry of bulk zinc polyphosphate glasses. Tribol Lett 48(3):393–406

    Article  Google Scholar 

  50. Xie Y, Chen M, Xie D, Zhong L, Zhang X (2017) A fast, low temperature zinc phosphate coating on steel accelerated by graphene oxide. Corros Sci 128:1–8

    Article  Google Scholar 

  51. Chen XF, Da ZJ, Gong JH, Zhang HJ, Zhu YK, Yang JY, Yuan PQ, Yuan WK (2020) Demetallization of heavy oil through pyrolysis: A reaction kinetics analysis. AIChE Journal n/a (n/a):e17086

  52. Leonenko SV, Kudryavtsev SA, Glikina IM (2017) Study of catalytic cracking process of fuel oil to obtain components of motor fuels using aerosol nanocatalysis technology. Adsorpt Sci Technol 35(9–10):878–883

    Article  Google Scholar 

Download references

Acknowledgements

The project was supported by Science and Technology Innovation 2025 Major project of Ningbo [2018B10038], the Chair Professorship Program of Shandong University of Technology [117002] and the Natural Science Foundation of ShanDong Province [ZR2020MB130].

Author information

Authors and Affiliations

Authors

Corresponding authors

Correspondence to Qingyan Chu or Ming Wang.

Ethics declarations

Conflict of interest

The authors declare no conflict of interest.

Additional information

Publisher's Note

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

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Yang, H., Chu, Q., Wang, M. et al. A continuous high-efficient demetallization strategy for used lubricating oils resource utilization. J Mater Cycles Waste Manag 25, 863–872 (2023). https://doi.org/10.1007/s10163-022-01571-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10163-022-01571-x

Keywords

Navigation