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Title: Perspectives on the relationship between materials chemistry and roll-to-roll electrode manufacturing for high-energy lithium-ion batteries

Journal Article · · Energy Storage Materials
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

As lithium-ion battery (LIB) active material and cell manufacturing costs continue to drop with wider adoption of electric vehicles, electrode and cell processing costs remain too high in terms of reaching the ultimate U.S. Department of Energy (DOE) cell cost target of $80/kWh. This paper primarily covers major materials chemistry advancements made over the last 10 years at Oak Ridge National Laboratory (ORNL) in the space of advanced manufacturing science for LIBs with the aim of simultaneously meeting the ultimate cost target, 500 Wh/kg gravimetric energy density, 10-15-min fast charge times, and 1000 deep discharge cycles. Aqeous electrode processing with a variety of active anode and cathode materials is now a standard procedure at the DOE Battery Manufacturing R&D Facility at ORNL (BMF), including the latest processes developed for Ni-rich cathodes. New results on cobalt-free LiNi0.8Fe0.1Al0.1O2 (NFA 811) are also included and discussed in an electrode processing advantage context. In addition, colloidal processing advancements have been made for Si/C composite anodes for achieving >600 mA h/g capacities. Optimization of electrode coating parameters and drying protocols have been completed, which has elucidated how key processing variables need to be changed when parameters such as slurry solids loading, solvent type, and wet electrode thickness are changed. ORNL has also increased the line speeds at which thick cathodes can be processed using ultra-fast electron beam (EB) curing and substantially decreased formation cycling times to <1 day. Finally, key details of these advancements are discussed in the context of materials chemistry and process-property-performance relationships.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1630512
Alternate ID(s):
OSTI ID: 1618989
Journal Information:
Energy Storage Materials, Vol. 29, Issue C; ISSN 2405-8297
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (64)

Materials processing for lithium-ion batteries journal March 2011
Prospects for reducing the processing cost of lithium ion batteries journal February 2015
Manufacturing energy analysis of lithium ion battery pack for electric vehicles journal January 2017
Energy impact of cathode drying and solvent recovery during lithium-ion battery manufacturing journal August 2016
Non-destructive evaluation of slot-die-coated lithium secondary battery electrodes by in-line laser caliper and IR thermography methods journal January 2014
Effect of electrode manufacturing defects on electrochemical performance of lithium-ion batteries: Cognizance of the battery failure sources journal April 2016
Fast formation cycling for lithium ion batteries journal February 2017
Solvent-Free Manufacturing of Electrodes for Lithium-ion Batteries journal March 2016
Understanding Interfacial-Energy-Driven Dry Powder Mixing for Solvent-Free Additive Manufacturing of Li-Ion Battery Electrodes journal September 2017
Solvent-free dry powder coating process for low-cost manufacturing of LiNi1/3Mn1/3Co1/3O2 cathodes in lithium-ion batteries journal June 2017
Analysis of electrolyte imbibition through lithium-ion battery electrodes journal June 2019
Electrode manufacturing for lithium-ion batteries—Analysis of current and next generation processing journal October 2019
Optimization of LiFePO 4 Nanoparticle Suspensions with Polyethyleneimine for Aqueous Processing journal February 2012
Towards water based ultra-thick Li ion battery electrodes – A binder approach journal May 2019
Water based processing of LiFePO4/C cathode material for Li-ion batteries utilizing freeze granulation journal September 2012
Enabling aqueous processing for crack-free thick electrodes journal June 2017
Water-based LiNi1/3Mn1/3Co1/3O2-cathodes with good electrochemical performance by use of additives journal January 2018
Chemical stability and long-term cell performance of low-cobalt, Ni-Rich cathodes prepared by aqueous processing for high-energy Li-Ion batteries journal January 2020
Superior Performance of LiFePO 4 Aqueous Dispersions via Corona Treatment and Surface Energy Optimization journal January 2012
Towards Understanding of Cracking during Drying of Thick Aqueous-Processed LiNi 0.8 Mn 0.1 Co 0.1 O 2 Cathodes journal February 2020
Chemical Weathering of Layered Ni-Rich Oxide Electrode Materials: Evidence for Cation Exchange journal January 2017
Method Using Water-Based Solvent to Prepare Li 7 La 3 Zr 2 O 12 Solid Electrolytes journal April 2018
Excellent Stability of a Lithium-Ion-Conducting Solid Electrolyte upon Reversible Li + /H + Exchange in Aqueous Solutions journal October 2014
Effect of Li+/H+ exchange in water treated Ta-doped Li7La3Zr2O12 journal September 2016
Corrosion of aluminum electrodes in aqueous slurries for lithium-ion batteries journal January 2014
Effect of aqueous-based cathode slurry pH and immersion time on corrosion of aluminum current collector in lithium-ion batteries: Effect of aqueous-based slurry on corrosion of aluminum journal April 2016
Enabling aqueous binders for lithium battery cathodes – Carbon coating of aluminum current collector journal February 2014
The high-temperature and high-humidity storage behaviors and electrochemical degradation mechanism of LiNi0.6Co0.2Mn0.2O2 cathode material for lithium ion batteries journal September 2017
On the Surface Chemistry of LiMO[sub 2] Cathode Materials (M=[MnNi] and [MnNiCo]): Electrochemical, Spectroscopic, and Calorimetric Studies journal January 2010
Studies on Storage Characteristics of LiNi[sub 0.4]Co[sub 0.2]Mn[sub 0.4]O[sub 2] as Cathode Materials in Lithium-Ion Batteries journal January 2007
Effect of Ambient Storage on the Degradation of Ni-Rich Positive Electrode Materials (NMC811) for Li-Ion Batteries journal January 2018
Washing effects on electrochemical performance and storage characteristics of LiNi0.8Co0.1Mn0.1O2 as cathode material for lithium-ion batteries journal January 2013
In Situ Coating of Li[Ni 0.33 Mn 0.33 Co 0.33 ]O 2 Particles to Enable Aqueous Electrode Processing journal April 2016
Technical and economic analysis of solvent-based lithium-ion electrode drying with water and NMP journal August 2017
On-Demand Hydrogen Generation using Nanosilicon: Splitting Water without Light, Heat, or Electricity journal January 2013
Si Oxidation and H 2 Gassing During Aqueous Slurry Preparation for Li-Ion Battery Anodes journal April 2018
Partially Oxidized Silicon Particles for Stable Aqueous Slurries and Practical Large-Scale Making of Si-Based Electrodes journal January 2015
Silicon Nanoparticles: Stability in Aqueous Slurries and the Optimization of the Oxide Layer Thickness for Optimal Electrochemical Performance journal September 2017
Nanosilicon Electrodes for Lithium-Ion Batteries: Interfacial Mechanisms Studied by Hard and Soft X-ray Photoelectron Spectroscopy journal February 2012
Quantifying gas generation from slurries used in fabrication of Si-containing electrodes for lithium-ion cells journal August 2018
What makes lithium substituted polyacrylic acid a better binder than polyacrylic acid for silicon-graphite composite anodes? journal April 2018
Unveiling the Role of Al 2 O 3 in Preventing Surface Reconstruction During High-Voltage Cycling of Lithium-Ion Batteries journal January 2019
Identifying the limiting electrode in lithium ion batteries for extreme fast charging journal December 2018
Modification of Ni-Rich FCG NMC and NCA Cathodes by Atomic Layer Deposition: Preventing Surface Phase Transitions for High-Voltage Lithium-Ion Batteries journal May 2016
Transition Metal Dissolution, Ion Migration, Electrocatalytic Reduction and Capacity Loss in Lithium-Ion Full Cells journal December 2016
Selecting the Best Graphite for Long-Life, High-Energy Li-Ion Batteries journal January 2018
Evaluation of Gas Formation and Consumption Driven by Crossover Effect in High-Voltage Lithium-Ion Batteries with Ni-Rich NMC Cathodes journal October 2019
Binder migration during drying of lithium-ion battery electrodes: Modelling and comparison to experiment journal July 2018
Evaluation Residual Moisture in Lithium-Ion Battery Electrodes and Its Effect on Electrode Performance journal January 2016
Drying and moisture resorption behaviour of various electrode materials and separators for lithium-ion batteries journal October 2017
High-Speed Fabrication of Lithium-Ion Battery Electrodes by UV-Curing journal April 2015
Electron Beam Curing of Composite Positive Electrode for Li-Ion Battery journal January 2016
Understanding limiting factors in thick electrode performance as applied to high energy density Li-ion batteries journal February 2017
Optimizing Areal Capacities through Understanding the Limitations of Lithium-Ion Electrodes journal November 2015
High–Speed electron beam curing of thick electrode for high energy density Li-ion batteries journal October 2019
Role of oxygen in polymerization reactions journal March 1991
A review of the features and analyses of the solid electrolyte interphase in Li-ion batteries journal September 2010
The state of understanding of the lithium-ion-battery graphite solid electrolyte interphase (SEI) and its relationship to formation cycling journal August 2016
Identifying the components of the solid–electrolyte interphase in Li-ion batteries journal August 2019
Surface properties of fluoroethylene carbonate-derived solid electrolyte interface on graphite negative electrode by narrow-range cycling in cell formation process journal December 2014
Micromechanisms of solid electrolyte interphase formation on electrochemically cycled graphite electrodes in lithium-ion cells journal December 2012
Balancing formation time and electrochemical performance of high energy lithium-ion batteries journal October 2018
Formation Challenges of Lithium-Ion Battery Manufacturing journal December 2019
On Leakage Current Measured at High Cell Voltages in Lithium-Ion Batteries journal December 2016