Journal
ADVANCED ENERGY MATERIALS
Volume 11, Issue 41, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202102421
Keywords
cobalt- and manganese-free cathodes; electrolyte-electrode interphases; high-nickel layered oxides; lithium-ion batteries; thermal stability
Categories
Funding
- Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) [DE-EE0007762]
- National Science Foundation Major Research Instrumentation (MRI) Award [1827608]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1827608] Funding Source: National Science Foundation
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This study presents a cobalt- and manganese-free ultrahigh-nickel LiNi0.93Al0.05Ti0.01Mg0.01O2 (NATM) cathode that demonstrates high capacity retention and enhanced thermal stability, outperforming common high-nickel cathodes.
High-nickel LiNi1-x-yMnxCoyO2 and LiNi1-x-yCoxAlyO2 cathodes are receiving growing attention due to the burgeoning demands on high-energy-density lithium-ion batteries. The presence of both cobalt and manganese in them, however, triggers multiple issues, including high cost, high toxicity, rapid surface deterioration, and severe transition-metal dissolution. Herein, a Co- and Mn-free ultrahigh-nickel LiNi0.93Al0.05Ti0.01Mg0.01O2 (NATM) cathode that exhibits 82% capacity retention over 800 deep cycles in full cells, outperforming two representative high-Ni cathodes LiNi0.94Co0.06O2 (NC, 52%) and LiNi0.90Mn0.05Co0.05O2 (NMC, 60%) is presented. It is demonstrated that a titanium-enriched surface along with aluminum and magnesium as the stabilizing ions in NATM not only ameliorates unwanted side reactions with the electrolyte and structural disintegrity, but also mitigates transition-metal dissolution and active lithium loss on the graphite anode. As a result, the graphite anode paired with NATM displays an ultrathin (approximate to 8 nm), monolayer anode-electrolyte interphase architecture after extensive cycling. Furthermore, NATM displays considerably enhanced thermal stability with an elevated exothermic temperature (213 degrees C for NATM vs 180 and 190 degrees C for NC and NMC, respectively) and remarkably reduced heat release. This work sheds light on rational compositional design to adopt ultrahigh-Ni cathodes in lithium-based batteries with low cost, long service life, and improved thermal stability.
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