Structure–performance relationships of lithium-ion battery cathodes revealed by contrast-variation small-angle neutron scattering

Liu, Qingsong; Brenneis, Willa; Nagy, Gergely; Doucet, Mathieu; Lopez, Jeffrey; Richards, Jeffrey J.

doi:10.1039/d4ta06364c

Title: Structure–performance relationships of lithium-ion battery cathodes revealed by contrast-variation small-angle neutron scattering

Journal Article · 22 October 2024 · Journal of Materials Chemistry. A

DOI: https://doi.org/10.1039/d4ta06364c · OSTI ID:2476709

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Northwestern Univ., Evanston, IL (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Lithium-ion battery cathodes are porous composites of active material, conductive carbon, and polymer binder. Controlling the cathode microstructure is key to achieving high energy density and cycling stability. Current characterization techniques lack the nanoscale resolution over representative volumes necessary to relate cathode microstructure to cycling performance. To address this challenge, we utilize contrast-variation small-angle neutron scattering to quantify the chemical and structural features of cathodes wet by dimethyl carbonate, representing a relevant solvent environment. Using neutron scattering measurements, we identify an expansion in carbon and polymer structures that arises after calendering and wetting with solvent. Further, we deconvolute the carbon and binder phases to obtain the solvent-accessible carbon black surface area, which we correlate to diminished capacity retention driven by electrolyte decomposition on exposed carbon. This technique provides nanoscale insight into composite cathode microstructures and resulting cycling performance, promising future applications to a broad range of porous materials that exist in energy storage systems.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725; SC0022119

OSTI ID:: 2476709

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 47 Vol. 12; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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