과황산계 산화제에 따른 폐LiFePO4 양극재에서 리튬의 침출 효과와 선택적 회수에 대한 연구
A Study on the Leaching Effect and Selective Recovery of Lithium Element by Persulfate-based Oxidizing Agents from Waste LiFePO4 Cathode
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초록
폐LiFePO4 배터리의 양극재에는 리튬이 약 4% 함유되어 있으며, 함유된 원소의 재활용은 환경적인 문제뿐만 아니라 자원순환의 관점에서 중요하다. 폐LiFePO4 양극재 분말에 함유된 리튬을 선택적으로 침출하기 위하여 3종류의 과황산계 산화제 [과황산나트륨(Na2S2O8), 과황산칼륨(K2S2O8), 그리고 과황산암모늄((NH4)2S2O8)]를 사용하여 각 성분의 침출율 및 분말특성을 비교 분석하였다. 침출시 광액농도를 변수로 두고 각 조건별로 3시간 동안 침출을 진행하였으며, 얻어진 침출용액은 ICP 성분분석을 시행하여 침출율을 계산하였다. 본 연구에서 사용된 모든 과황산계 산화제 종류에서 92% 이상의 리튬 침출율을 보였다. 특히 과황산암모늄의 산화제를 사용하여침출하였을 경우, 50 g/L의 광액농도 및 1.1 몰 비의 산화제 농도에서 약 93.3%의 가장 높은 리튬의 침출율을 보였다.
Abstract
In waste lithium iron phosphate (LFP) batteries, the cathode material contains approximately 4% lithium. Recycling the constituent elements of batteries is important for resource circulation and for mitigating the environmental pollution. Li contained in the waste LFP cathode powder was selectively leached using persulfate-based oxidizing agents, such as sodium persulfate, potassium persulfate, and ammonium persulfate. Leaching efficiency and waste LFP powder properties were compared and analyzed. Pulp density was used as a variable during leaching, which was performed for 3 h under each condition. The leaching efficiency was calculated using the inductively coupled plasma (ICP) analysis of the leachate. All types of persulfate-based oxidizing agents used in this study showed a Li leaching efficiency over 92%. In particular, when leaching was performed using (NH4)2S2O8, the highest Li leaching percentage of 93.3% was observed, under the conditions of 50 g/L pulp density and an oxidizing agent concentration of 1.1 molar ratio.
참고문헌 (40)
- Xie, J., "A retrospective on lithium-ion batteries", Nature Communications, 11(1), pp.2499~ (2020)
- Kim, H., "Electric vehicle battery recycling industry trends and implications", pp.4~38 (2022), Institute for International Trade
- Zeng, X., "Solving spent lithium-ion battery problems in China : Opportunities and challenges", Renewable and Sustainable Energy Reviews, 52, pp.1759~1767 (2015)
- Natarajan, S., "Recycling strategies for spent Li-ion battery mixed cathodes", ACS Energy Letters, 3(9), pp.2101~2103 (2018)
- Padhi, A. K., "Effect of structure on the Fe3+", Fe2+ redox couple in iron phosphates, 1997, pp.144(5), 1609~
- Zeng, X., "Com-mercialization of lithium battery technologies for electric vehicles", Advanced Energy Materials, 9(27), pp.1900161~ (2019)
- Jing, Q., "Direct regeneration of spent LiFePO4 cathode material by a green and efficient one-step hydrothermal method", ACS Sustainable Chemistry & Engineering, 8(48), pp.17622~17628 (2020)
- 박은미, "건식 공정을 통한 리튬이차전지의 재활용 연구 동향", 자원리싸이클링, 31(3), pp.27~39 (2022), 한국자원리싸이클링학회[DOI]
- 주소영, "폐리튬이차전지에서 회수된 황산리튬 전구체로부터 침전제 종류별 수산화리튬 제조 거동 연구", 자원리싸이클링, 30(1), pp.44~52 (2021), 한국자원리싸이클링학회[DOI]
- 김대원, "리튬 함유 물질로부터 탄산리튬 회수에 대한 고찰", 한국결정성장학회지, 29(3), pp.91~106 (2019), 한국결정성장학회[DOI]
- 양재교, "탄산리튬 분말 제조에 있어서 탄산화 반응에 관한 연구", 한국결정성장학회지, 29(5), pp.222~228 (2019), 한국결정성장학회[DOI]
- 진연호, "리튬 함유 폐액에서의 리튬 농도와 생태독성과의 연관성 연구", Clean Technology, 27(1), pp.33~38 (2021), 한국청정기술학회
- 김보람, "폐리튬이차전지 스크랩 재활용을 통한 양극활물질 전구체 합성 연구", 한국결정성장학회지, 32(2), pp.61~67 (2022), 한국결정성장학회[DOI]
- 정연재, "폐 배터리 셀 분말의 선택적 리튬 침출을 위한 질산염화 공정 최적화 연구", 자원리싸이클링, 30(6), pp.43~52 (2021), 한국자원리싸이클링학회[DOI]
- Yu, X., "Achieving low-temperature hydrothermal relithiation by redox mediation for direct recycling of spent lithium-ion battery cathodes", Energy Storage Materials, 51, pp.54~62 (2022)
- 문현승, "황산용액에서 용매추출에 의한 코발트(II), 니켈(II) 및 구리(II) 분리", 자원리싸이클링, 31(1), pp.21~28 (2022), 한국자원리싸이클링학회[DOI]
- Chen, J., "Environmentally friendly recycling and effective repairing of cathode powders from spent LiFePO4 batteries", Green Chem, 18(8), pp.2500~2506 (2016)
- Song, X., "Direct regeneration of cathode materials from spent lithium iron phosphate batteries using a solid phase sintering method", RSC Adv, 7(8), pp.4783~4790 (2017)
- Li, X., "Direct regeneration of recycled cathode material mixture from scrapped LiFePO4 batteries", J. Power Sources, 345, pp.78~84 (2017)
- Zhang, X., "Sustainable re-cycling and regeneration of cathode scraps from industrial production of lithium-ion batteries", ACS Sustainable Chem. Eng, 4(12), pp.7041~7049 (2016)
- Li, H., "Recovery of Lithium, Iron, and Phosphorus from Spent LiFePO4 Batteries Using Stoichiometric Sulfuric Acid Leaching System", ACS Sus-tainable Chem. Eng, 5, pp.8017~8024 (2017)
- Cai, G., "Process Development for the Recycle of Spent Lithium Ion Batteries by Chemical Precipitation", Ind. Eng. Chem. Res, 53(47), pp.18245~18259 (2014)
- Mahandra, H., "A sustainable process for selective recovery of lithium as lithium phosphate from spent LiFePO4 batteries", Resources, Conservation & Re-cycling, 175, pp.105883~ (2021)
- Kumar, J., "Selective recovery of Li and FePO4 from spent LiFePO4 cathode scraps by organic acids and the properties of the regenerated LiFePO4", Waste Management, 113, pp.32~40 (2020)
- Yang, Y., "Selective recovery of lithium from spent lithium iron phosphate batteries : a sustainable process", Green Chem, 20(13), pp.3121~3133 (2018)
- Zhang, J., "Sustainable and Facile Method for the Selective Recovery of Lithium from Cathode Scrap of Spent LiFePO4 Batteries", ACS Sustain. Chem. Eng, 7(6), pp.5626~5631 (2019)
- Bian, D., "A novel process to recycle spent LiFePO4 for synthesizing LiFePO4", C hierar-chical microflowers, 2016, pp.190, 134~140
- Huang, Y., "A stepwise recovery of metals from hybrid cathodes of spent Li-ion batteries with leaching-flotation-precipitation process", Journal of Power Sources, 325, pp.555~564 (2016)
- Kumar, J., "Selective recovery of Li and FePO4 from spent LiFePO4 cathode scraps by organic acids and the properties of the regenerated LiFePO4", Waste Management, 113, pp.32~40 (2020)
- Li, L., "A green and effective room-temperature recycling process of LiFePO4cathode materials for lithium-ion batteries", Waste Mana-gement, 85, pp.437~444 (2019)
- Fan, E., "Selective recovery of Li and Fe from spent lithium-ion batteries by an environmentally friendly mechanochemical approach", ACS Sustainable Chemistry & Engineering, 6(8), pp.11029~11035 (2018)
- Liu, K., "Selective extraction of lithium from a spent lithium iron phosphate battery by mechanochemical solid-phase oxidation", Green Chemistry, 23(3), pp.1344~1352 (2021)
- Peng, D., "Closed-loop regeneration of LiFePO4 from spent lithium-ion batteries : A"feed three birds with one scone"strategy toward advanced cathode materials", Journal of Cleaner Production, 316, pp.128098~ (2021)
- Tao, S., "A method for re-covering Li3PO4 from spent lithium iron phosphate cathode material through high-temerature activation", Ionics, 25, pp.5643~5653 (2019)
- Ji, G., "Efficient utilization of scrapped LiFePO4 battery for novel synthesis of Fe2P2O7", C as candidate anode materals, 2021, pp.174, 105802~
- Janssen, Y., "Reciprocal Salt Flux Growth of LiFePO4 Single Crystals with Controlled Defect Concentrations", Chem. Mater, 25, pp.4574~ (2013)
- Gangaja, B., "Reuse, recycle, and regeneration of LiFePO4 cathode from spent lithium-ion batteries for rechargeable lithium-and sodium-ion batteries", ACS Sustainable Chemistry & Engineering, 9(13), pp.4711~4721 (2021)
- SIDS Initial Assessment Report For SIAM 20 Paris, , 19~21 (2005)
- Balej, J., "Mean Activity Coefficients of Peroxo-disulfates in Saturated Solutions of the Conversion System 2NH—2Na—SO—SO—HO at 20℃ and 30℃", Acta Chimica Slovaca, 6(2), pp.163~167 (2013)
- Apelblat, A., "Solubilities and vapour pressures of saturated aqueous solutions of sodium peroxydisulfate and potassium peroxydisulfate", The Journal of Chemical Thermodynamics, 33(1), pp.61~69 (2001)
