Electrolyte-induced surface transformation and transition-metal dissolution of fully delithiated LiNi0.8Co0.15Al0.05O2

Faenza, Nicholas V.; Lebens-Higgins, Zachary W.; Mukherjee, Pinaki; Sallis, Shawn; Pereira, Nathalie; Badway, Fadwa; Halajko, Anna; Ceder, Gerbrand; Cosandey, Frederic; Piper, Louis. F. J.; Amatucci, Glenn G.

doi:10.1021/acs.langmuir.7b00863

Title: Electrolyte-induced surface transformation and transition-metal dissolution of fully delithiated LiNi_0.8Co_0.15Al_0.05O₂

Journal Article · Thu Jun 08 00:00:00 EDT 2017 · Langmuir

DOI: https://doi.org/10.1021/acs.langmuir.7b00863 · OSTI ID:1364759

^[1]; Lebens-Higgins, Zachary W. ^[2]; Mukherjee, Pinaki ^[3]; Sallis, Shawn ^[2]; Pereira, Nathalie ^[4]; Badway, Fadwa ^[4]; Halajko, Anna ^[4]; Ceder, Gerbrand ^[5]; Cosandey, Frederic ^[3];

^[2];

^[4]

Rutgers Univ., North Brunswick, NJ (United States); Rutgers University
Binghamton Univ., Binghamton, NY (United States)
Rutgers Univ., Piscataway, NJ (United States)
Rutgers Univ., North Brunswick, NJ (United States)
Univ. of California, Berkeley, CA (United States)

Here, enabling practical utilization of layered R$$\bar{3}$$m positive electrodes near full delithiation requires an enhanced understanding of the complex electrode–electrolyte interactions that often induce failure. Using Li[Ni_0.8Co_0.15Al_0.05]O₂ (NCA) as a model layered compound, the chemical and structural stability in a strenuous thermal and electrochemical environment was explored. Operando microcalorimetry and electrochemical impedance spectroscopy identified a fingerprint for a structural decomposition and transition-metal dissolution reaction that occurs on the positive electrode at full delithiation. Surface-sensitive characterization techniques, including X-ray absorption spectroscopy and high-resolution transmission electron microscopy, measured a structural and morphological transformation of the surface and subsurface regions of NCA. Despite the bulk structural integrity being maintained, NCA surface degradation at a high state of charge induces excessive transition-metal dissolution and significant positive electrode impedance development, resulting in a rapid decrease in electrochemical performance. Additionally, the impact of electrolyte salt, positive electrode surface area, and surface Li₂CO₃ content on the magnitude and character of the dissolution reaction was studied.

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Research Organization:: Rutgers Univ., New Brunswick, NJ (United States); Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012583

OSTI ID:: 1364759

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 37 Vol. 33; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Electrolyte-induced surface transformation and transition-metal dissolution of fully delithiated LiNi0.8Co0.15Al0.05O2

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Title: Electrolyte-induced surface transformation and transition-metal dissolution of fully delithiated LiNi_0.8Co_0.15Al_0.05O₂