Environmentally Friendly Recycling of Lithium Ion Batteries

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dc.contributor.authorSonoc, Alexandruen
dc.contributor.departmentMechanical and Materials Engineeringen
dc.contributor.supervisorJeswiet, Jacob
dc.date.accessioned2020-06-02T21:38:50Z
dc.date.available2020-06-02T21:38:50Z
dc.degree.grantorQueen's University at Kingstonen
dc.description.abstractRecycling lithium ion batteries (LIBs) and using their recovered materials to make new ones has many economic, social, and environmental benefits. The greatest benefits come from recycling metals from cathode active materials (CAMs), for example Li, Ni, Co, and Mn from NCM111 (a common electric vehicle CAM). Hydrometallurgical recycling processes, in which CAMs are leached and metals are extracted from the pregnant leach solution (PLS), are favoured because they can recover all metals. Due to the hazards of leaching with strong acids, organic acids are becoming preferred lixiviants; however, they are expensive. In this work, two green chemistry hydrometallurgy processes were developed to recycle CAMs from LIBs. Both processes regenerate organic acid lixiviant, have high Li, Ni, Co, and Mn recoveries, and produce sodium-free Li2CO3. In the first process, Donnan Dialysis is used to extract Li, then Ni, Co, and Mn, as well as to reprotonate organic acid in PLS. Donnan Dialysis combined with bicarbonation and decarbonation is used to produce Li2CO3 from the Li extract. Heating is not required in the process. Mass balances, charge balances, and mass flux equations were developed. Experiments were performed to obtain mass transfer coefficients. The process was simulated and the results were: recoveries of 94.1% for Li and 99.4% for Ni, Co, and Mn and 98.9% of organic acid reprotonated. In the second process, formic acid was used to leach NCM111 while simultaneously precipitating Ni, Co, and Mn formate salts. These salts were reacted with sulphuric acid to yield mixed Ni, Co, and Mn sulphate salts and formic acid, which was evaporated. The PLS was saturated with Li2CO3, which precipitated residual Ni, Co, and Mn, and was filtered then dewatered. The LiCOOH salts obtained were thermally decomposed in air to 99.97 wt% Li2CO3. Recoveries of Li, Ni, Co, and Mn were 100%. The process produces neither solid nor liquid waste. By condensing vapours from dewatering and evaporation steps, 66% of the water and 57% of the formic acid needed for leaching can be recovered for reuse. Mixed Ni, Co, and Mn sulphate salts and Li2CO3 can be used to make new LIBs.en
dc.description.degreePhDen
dc.embargo.liftdate2025-06-02T08:14:00Z
dc.embargo.termsI request that my thesis be restricted until June 15, 2021. The second manuscript in the thesis has not been published yet. I would like to submit it to a quality journal and do not wish for it to be available to the public before it has been published. Additionally, my supervisors and I have filled a provisional patent for the process developed in the second manuscript. We intent to do additional work on it before filling a full patent in May, 2021. I trust that in the unlikely event the second manuscript is not yet published by June 15, 2021, I can ask for a longer extension and receive it.en
dc.identifier.urihttp://hdl.handle.net/1974/27883
dc.language.isoengen
dc.relation.ispartofseriesCanadian thesesen
dc.rightsQueen's University's Thesis/Dissertation Non-Exclusive License for Deposit to QSpace and Library and Archives Canadaen
dc.rightsProQuest PhD and Master's Theses International Dissemination Agreementen
dc.rightsIntellectual Property Guidelines at Queen's Universityen
dc.rightsCopying and Preserving Your Thesisen
dc.rightsThis publication is made available by the authority of the copyright owner solely for the purpose of private study and research and may not be copied or reproduced except as permitted by the copyright laws without written authority from the copyright owner.en
dc.subjectLithium Ion Batteriesen
dc.subjectRecyclingen
dc.subjectGreen Chemistryen
dc.subjectDonnan Dialysisen
dc.subjectFormic Aciden
dc.subjectSodium-Freeen
dc.subjectSodium-Free Li2CO3en
dc.subjectSodium-Free Lithium Carbonateen
dc.subjectZero Liquid Dischargeen
dc.subjectRecycling of Lithium Ion Batteriesen
dc.subjectBicarbonationen
dc.subjectDecarbonationen
dc.subjectNCM111en
dc.subjectNMC111en
dc.subjectThermal Decompositionen
dc.subjectThermal Decomposition of Lithium Formateen
dc.subjectThermal Decomposition of LiCOOHen
dc.subjectMixed Ni, Co, and Mn Sulphatesen
dc.subjectMixed Ni, Co, and Mn Sulfatesen
dc.subjectMixed Sulfatesen
dc.subjectLithiumen
dc.subjectNickelen
dc.subjectCobalten
dc.subjectManganeseen
dc.subjectFormateen
dc.subjectMixed Sulphatesen
dc.subjectZero Solid Wasteen
dc.subjectNo Liquid Wasteen
dc.subjectNo Solid Wasteen
dc.subjectEnvironmentally Friendly Recyclingen
dc.subjectOrganic Acid Lixivianten
dc.subjectOrganic Acid Leachingen
dc.subjectLeachingen
dc.subjectFormic Acid Leachingen
dc.titleEnvironmentally Friendly Recycling of Lithium Ion Batteriesen
dc.typethesisen
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