Towards Understanding of Cracking during Drying of Thick Aqueous-Processed LiNi0.8Mn0.1Co0.1O2 Cathodes

Sahore, Ritu; Wood, III, David L.; Kukay, Alexander; Grady, Kelsey M.; Li, Jianlin; Belharouak, Ilias

doi:10.1021/acssuschemeng.9b06363

Towards Understanding of Cracking during Drying of Thick Aqueous-Processed LiNi_0.8Mn_0.1Co_0.1O₂ Cathodes

Journal Article · Wed Feb 19 00:00:00 EST 2020 · ACS Sustainable Chemistry & Engineering

DOI:https://doi.org/10.1021/acssuschemeng.9b06363· OSTI ID:1606846

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Replacing N-methyl-2-pyrrolidone (NMP) with water for processing of lithium-ion battery (LIB) electrodes has both cost and environmental benefits, which include reduced drying time, lower dryer capital cost, elimination of NMP recovery capital equipment, and no release of volatile organic compounds (VOCs) into the environment. However, aqueous-processed thick cathodes (≳4 mAh/cm²) typically exhibit detrimental cracking during drying that is not observed for the NMP-based counterpart. The reasons for cracking of these water-based thick electrodes are still not well understood due to the complex nature of the colloidal dispersions used in the LIB electrode processing steps. In this work, the contributions of various factors responsible for cracking are discussed. We show that eliminating hydrogen evolution due to corrosion of the aluminum current collector eliminated the majority of the cracks regardless of the coating thickness, identifying the gas evolution as the primary reason for electrode cracking. Some secondary cracks and pinhole-type defects remained after addressing the aluminum current collector corrosion, which are thought to be caused by an inferior binding network formed by carbon black and binder in aqueous-processed cathodes compared to those processed with NMP. The thick aqueous processed cathodes are not able to sufficiently withstand the drying stresses without crack formation. We demonstrate reduction of these secondary defects by either improving the binding network or by reducing the drying stress. The former was achieved by replacing carbon black with vapor grown graphite tubes (VGGTs) that caused a more efficient utilization of the emulsion binder. Here, the latter was achieved by adding a small amount of IPA as a co-solvent that has been shown to reduce capillary stresses.

View Accepted Manuscript (DOE)

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:: 1606846

Journal Information:: ACS Sustainable Chemistry & Engineering, Journal Name: ACS Sustainable Chemistry & Engineering Journal Issue: 8 Vol. 8; ISSN 2168-0485

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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