Drying Temperature and Capillarity-Driven Crack Formation in Aqueous Processing of Li-Ion Battery Electrodes

Rollag, Kelsey; Juarez-Robles, Daniel; Du, Zhijia; Wood, David L.; Mukherjee, Partha P.

doi:10.1021/acsaem.9b00704

Title: Drying Temperature and Capillarity-Driven Crack Formation in Aqueous Processing of Li-Ion Battery Electrodes

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Abstract

Unlike conventional electrode processing for Li-ion batteries, which uses the expensive and highly toxic organic N-methyl-2-pyrrolidone (NMP) solvent, aqueous processing simply employs deionized water as the solvent. Yet, thick aqueous processed cathodes have been found to crack during drying. Here, the influence of electrode drying temperature and thickness on cracking was investigated. LiNi_1/3Mn_1/3Co_1/3O₂ cathodes prepared with a hydrophilic binder, modified styrene–butadiene rubber (SBR), were coated at various thicknesses and dried at temperatures ranging from 20 to 70 °C. Experiments revealed cracking worsens with increased electrode thickness and elevated drying temperatures. Cracks were formed during the capillarity-driven phase during drying. Strong evaporation and weak diffusion played a critical role in the nonuniform distribution of the inactive phase. Images of electrode surfaces were processed to quantify crack dimensions and crack intensity factor (CIF). The average crack length and width, as well as CIF, increased with drying temperature and electrode thickness. Electrochemical performance revealed a strong and negative correlation between the crack density and performance in terms of specific capacity. Transport limitations associated with the presence of cracks adversely affect the advantage of high volume ratio of active materials in the thick electrodes.

Authors:

Rollag, Kelsey ^[1]; Juarez-Robles, Daniel ^[2];

^[3];

^[2]

Texas A & M Univ., College Station, TX (United States)
Purdue Univ., West Lafayette, IN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Mon Jun 03 00:00:00 EDT 2019

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

OSTI Identifier:: 1530066

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: ACS Applied Energy Materials

Additional Journal Information:: Journal Volume: 2; Journal Issue: 6; Journal ID: ISSN 2574-0962

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 25 ENERGY STORAGE; aqueous processing; thick cathode; hydrophilic binder; drying temperature; capillarity; crack formation

Citation Formats


                    Rollag, Kelsey, Juarez-Robles, Daniel, Du, Zhijia, Wood, David L., and Mukherjee, Partha P. Drying Temperature and Capillarity-Driven Crack Formation in Aqueous Processing of Li-Ion Battery Electrodes.  United States: N. p., 2019. 
Web.  doi:10.1021/acsaem.9b00704.

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                    Rollag, Kelsey, Juarez-Robles, Daniel, Du, Zhijia, Wood, David L., & Mukherjee, Partha P. Drying Temperature and Capillarity-Driven Crack Formation in Aqueous Processing of Li-Ion Battery Electrodes.  United States.  https://doi.org/10.1021/acsaem.9b00704

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                    Rollag, Kelsey, Juarez-Robles, Daniel, Du, Zhijia, Wood, David L., and Mukherjee, Partha P. Mon .  
"Drying Temperature and Capillarity-Driven Crack Formation in Aqueous Processing of Li-Ion Battery Electrodes".  United States.  https://doi.org/10.1021/acsaem.9b00704.  https://www.osti.gov/servlets/purl/1530066.

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@article{osti_1530066,

  title        = {Drying Temperature and Capillarity-Driven Crack Formation in Aqueous Processing of Li-Ion Battery Electrodes},

  author       = {Rollag, Kelsey and Juarez-Robles, Daniel and Du, Zhijia and Wood, David L. and Mukherjee, Partha P.},

  abstractNote = {Unlike conventional electrode processing for Li-ion batteries, which uses the expensive and highly toxic organic N-methyl-2-pyrrolidone (NMP) solvent, aqueous processing simply employs deionized water as the solvent. Yet, thick aqueous processed cathodes have been found to crack during drying. Here, the influence of electrode drying temperature and thickness on cracking was investigated. LiNi1/3Mn1/3Co1/3O2 cathodes prepared with a hydrophilic binder, modified styrene–butadiene rubber (SBR), were coated at various thicknesses and dried at temperatures ranging from 20 to 70 °C. Experiments revealed cracking worsens with increased electrode thickness and elevated drying temperatures. Cracks were formed during the capillarity-driven phase during drying. Strong evaporation and weak diffusion played a critical role in the nonuniform distribution of the inactive phase. Images of electrode surfaces were processed to quantify crack dimensions and crack intensity factor (CIF). The average crack length and width, as well as CIF, increased with drying temperature and electrode thickness. Electrochemical performance revealed a strong and negative correlation between the crack density and performance in terms of specific capacity. Transport limitations associated with the presence of cracks adversely affect the advantage of high volume ratio of active materials in the thick electrodes.},

  doi          = {10.1021/acsaem.9b00704},

  journal      = {ACS Applied Energy Materials},

  number       = 6,

  volume       = 2,

  place        = {United States},

  year         = {Mon Jun 03 00:00:00 EDT 2019},

  month        = {Mon Jun 03 00:00:00 EDT 2019}

}

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