Thermally-driven mesopore formation and oxygen release in delithiated NCA cathode particles

Besli, Münir M.; Shukla, Alpesh Khushalchand; Wei, Chenxi; Metzger, Michael; Alvarado, Judith; Boell, Julian; Nordlund, Dennis; Schneider, Gerhard; Hellstrom, Sondra; Johnston, Christina; Christensen, Jake; Doeff, Marca M.; Liu, Yijin; Kuppan, Saravanan

doi:10.1039/c9ta01720h

Title: Thermally-driven mesopore formation and oxygen release in delithiated NCA cathode particles

Journal Article · Wed Apr 24 00:00:00 EDT 2019 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/c9ta01720h· OSTI ID:1547284

^[1];

^[2]; Wei, Chenxi ^[3];

^[4]; Alvarado, Judith ^[5]; Boell, Julian ^[4]; Nordlund, Dennis ^[3]; Schneider, Gerhard ^[6]; Hellstrom, Sondra ^[4]; Johnston, Christina ^[4];

^[4];

^[5];

^[3];

^[4]

Robert Bosch LLC, Sunnyvale, CA (United States); Karlsruhe Inst. of Technology (KIT) (Germany)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Robert Bosch LLC, Sunnyvale, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Karlsruhe Inst. of Technology (KIT) (Germany); Aalen Univ. (Germany)

The structural integrity of layered Ni-rich oxide cathode materials is one of the most significant factors that critically affect the performance and reliability of lithium-ion batteries. Prolonged battery operation many times involves repeated phase transitions, buildup of mechanical stresses, and could provoke thermal spikes. Such sophisticated chemo-thermo-mechanical interplay can cause performance degradation through structural disintegration of the cathode active materials (CAMs). In this work, we systematically investigate the thermal decomposition, fracture, and oxygen evolution of chemically delithiated Li_0.3Ni_0.8Co_0.15Al_0.05O₂ (NCA) particles upon heating from 25 °C to 450 °C using a number of advanced X-ray and electron probes. We observed a continuous reduction of the Ni oxidation state upon heating, as well as the release of oxygen from the NCA lattice that undergoes the thermally induced phase transformations. The release of oxygen also created numerous mesopores throughout the analyzed particles, which could significantly affect the chemical and mechanical properties of the electrode. In addition, intergranular and intragranular fracturing at elevated temperatures also contribute to the degradation of the NCA cathode under these conditions. Our investigation of the mechanical integrity at elevated temperatures provides a fundamental understanding of the thermally driven chemomechanical breakdown of the NCA cathode active materials.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515

OSTI ID:: 1547284

Alternate ID(s):: OSTI ID: 1511062; OSTI ID: 1581069

Journal Information:: Journal of Materials Chemistry. A, Vol. 7, Issue 20; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 39 works

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