Enabling Aqueous Processing for LiNi 0.5 Mn 1.5 O 4 ‐Based Positive Electrodes in Lithium‐Ion Batteries by Applying Lithium‐Based Processing Additives

pH value in the electrode paste, thereby corroding the aluminum current collector. Herein, the in fl uence of different lithium salts as processing additive to tailor the pH value of the electrode paste, the manganese dissolution during processing, and the electrochemical performance is described for aqueous processing of LiNi 0.5 Mn 1.5 O 4 -based positive electrodes. Positive electrodes, based on an aqueous LiNi 0.5 Mn 1.5 O 4 -based electrode paste which is mixed with LiN(SO 2 CF 3 ) 2 (LiTFSI), achieve a comparable electrochemical performance to state-of-the-art nonaqueous-processed electrodes. Manganese dissolution into the electrode paste is examined by inductively coupled plasma-mass spectrometry (ICP-MS), showing that the addition of lithium salts to the electrode paste substantially decreases manganese leaching during processing. Furthermore, postmortem analysis shows that the addition of LiTFSI to the electrode paste has a positive effect not only during processing but also on charge/discharge cycling performance.

[1]  M. Winter,et al.  The role of the pH value in water-based pastes on the processing and performance of Ni-rich LiNi0.5Mn0.3Co0.2O2 based positive electrodes , 2020 .

[2]  G. Giffin,et al.  Implications of Aqueous Processing for High Energy Density Cathode Materials: Part I. Ni-Rich Layered Oxides , 2020 .

[3]  G. Giffin,et al.  Surface Modification of LiNi0.8Co0.15Al0.05O2 Particles via Li3PO4 Coating to Enable Aqueous Electrode Processing , 2020, ChemSusChem.

[4]  D. Wood,et al.  Aqueous Ni-rich-cathode dispersions processed with phosphoric acid for lithium-ion batteries with ultra-thick electrodes. , 2020, Journal of colloid and interface science.

[5]  D. Wood,et al.  Lithium and transition metal dissolution due to aqueous processing in lithium-ion battery cathode active materials , 2020 .

[6]  M. Winter,et al.  Toward Green Battery Cells: Perspective on Materials and Technologies , 2020 .

[7]  D. Wood,et al.  Water-Based Electrode Manufacturing and Direct Recycling of Lithium-Ion Battery Electrodes—A Green and Sustainable Manufacturing System , 2020, iScience.

[8]  D. Wood,et al.  Analysis of electrolyte imbibition through lithium-ion battery electrodes , 2019, Journal of Power Sources.

[9]  M. Winter,et al.  Towards water based ultra-thick Li ion battery electrodes – A binder approach , 2019, Journal of Power Sources.

[10]  Ahmad T. Mayyas,et al.  The case for recycling: Overview and challenges in the material supply chain for automotive li-ion batteries , 2019, Sustainable Materials and Technologies.

[11]  M. Winter,et al.  Before Li Ion Batteries. , 2018, Chemical reviews.

[12]  Xiqian Yu,et al.  Dynamic evolution of cathode electrolyte interphase (CEI) on high voltage LiCoO2 cathode and its interaction with Li anode , 2018, Energy Storage Materials.

[13]  J. Prausnitz,et al.  Solubilities of six lithium salts in five non-aqueous solvents and in a few of their binary mixtures , 2018 .

[14]  M. Winter,et al.  Performance and cost of materials for lithium-based rechargeable automotive batteries , 2018 .

[15]  Partha P. Mukherjee,et al.  Enabling aqueous processing for crack-free thick electrodes , 2017 .

[16]  James A. Gilbert,et al.  Chemical Weathering of Layered Ni-Rich Oxide Electrode Materials: Evidence for Cation Exchange , 2017 .

[17]  Emilie Bekaert,et al.  Effects of Biphenyl Polymerization on Lithium Deposition in Commercial Graphite/NMC Lithium-Ion Pouch-Cells during Calendar Aging at High Temperature , 2017 .

[18]  S. Passerini,et al.  Graphite//LiNi0.5 Mn1.5 O4 Cells Based on Environmentally Friendly Made-in-Water Electrodes. , 2017, ChemSusChem.

[19]  E. Peled,et al.  Review—SEI: Past, Present and Future , 2017 .

[20]  R. Behm,et al.  Complementary strategies towards the aqueous processing of high-voltage LiNi , 2017 .

[21]  M. Winter,et al.  Best Practice: Performance and Cost Evaluation of Lithium Ion Battery Active Materials with Special Emphasis on Energy Efficiency , 2016 .

[22]  M. Winter,et al.  Comparison of Different Synthesis Methods for LiNi0.5Mn1.5O4—Influence on Battery Cycling Performance, Degradation, and Aging , 2016 .

[23]  G. G. Eshetu,et al.  In-Depth Interfacial Chemistry and Reactivity Focused Investigation of Lithium-Imide- and Lithium-Imidazole-Based Electrolytes. , 2016, ACS applied materials & interfaces.

[24]  M. Winter,et al.  Investigations on the C-Rate and Temperature Dependence of Manganese Dissolution/Deposition in LiMn2O4/Li4Ti5O12 Lithium Ion Batteries , 2016 .

[25]  K. Ahn,et al.  Stress Development of Li-Ion Battery Anode Slurries during the Drying Process , 2015 .

[26]  A. Eddahech,et al.  Determination of lithium-ion battery state-of-health based on constant-voltage charge phase , 2014 .

[27]  S. Bodoardo,et al.  Enabling aqueous binders for lithium battery cathodes - Carbon coating of aluminum current collector , 2014 .

[28]  Stefano Passerini,et al.  Performance of LiNi1/3Mn1/3Co1/3O2/graphite batteries based on aqueous binder , 2014 .

[29]  Dong Zhang,et al.  Enhanced electrochemical properties of TiO2(B) nanoribbons using the styrene butadiene rubber and sodium carboxyl methyl cellulose water binder , 2014 .

[30]  Jun Lu,et al.  Mn(II) deposition on anodes and its effects on capacity fade in spinel lithium manganate–carbon systems , 2013, Nature Communications.

[31]  M. Winter,et al.  Investigation of different binding agents for nanocrystalline anatase TiO2 anodes and its application in a novel, green lithium-ion battery , 2013 .

[32]  M. Winter,et al.  Natural cellulose as binder for lithium battery electrodes , 2012 .

[33]  S. Passerini,et al.  Investigations on cellulose-based high voltage composite cathodes for lithium ion batteries , 2011 .

[34]  Alain Mauger,et al.  Aging of LiNi1/3Mn1/3Co1/3O2 cathode material upon exposure to H2O , 2011 .

[35]  M. Winter,et al.  Low Cost, Environmentally Benign Binders for Lithium-Ion Batteries , 2010 .

[36]  Martin Winter,et al.  The Solid Electrolyte Interphase – The Most Important and the Least Understood Solid Electrolyte in Rechargeable Li Batteries , 2009 .

[37]  T. Gustafsson,et al.  A comparative XPS surface study of Li2FeSiO4/C cycled with LiTFSI- and LiPF6-based electrolytes , 2009 .

[38]  P. Novák,et al.  Study of styrene butadiene rubber and sodium methyl cellulose as binder for negative electrodes in lithium-ion batteries , 2006 .

[39]  Young-Min Choi,et al.  Aqueous processing of natural graphite particulates for lithium-ion battery anodes and their electrochemical performance , 2005 .

[40]  Christopher S. Johnson,et al.  Lithium and Deuterium NMR Studies of Acid-Leached Layered Lithium Manganese Oxides , 2002 .

[41]  M. Wagner,et al.  The effect of the binder morphology on the cycling stability of Li–alloy composite electrodes , 2001 .

[42]  Deborah J. Jones,et al.  Ion Exchange in Manganese Dioxide Spinel: Proton, Deuteron, and Lithium Sites Determined from Neutron Powder Diffraction Data , 1998 .

[43]  W. F. Howard,et al.  M3+-modified LiMn2O4 spinel intercalation cathodes: I. Admetal effects on morphology and electrochemical performance , 1997 .

[44]  Seung M. Oh,et al.  Electrolyte Effects on Spinel Dissolution and Cathodic Capacity Losses in 4 V Li / Li x Mn2 O 4 Rechargeable Cells , 1997 .

[45]  J. C. Hunter.  Preparation of a new crystal form of manganese dioxide: λ-MnO2 , 1981 .

[46]  Emanuel Peled,et al.  The Electrochemical Behavior of Alkali and Alkaline Earth Metals in Nonaqueous Battery Systems—The Solid Electrolyte Interphase Model , 1979 .