4.8 Article

Constructing a Protective Pillaring Layer by Incorporating Gradient Mn4+ to Stabilize the Surface/Interfacial Structure of LiNi0.815Co0.15Al0.035O2 Cathode

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 10, Issue 33, Pages 27821-27830

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b10372

Keywords

Lithium-ion batteries; NCA; surface modification; gradient concentration; NiO-like phase; pillar effect; structure stability

Funding

  1. National Natural Science Foundation of China [21506133]
  2. Youth Foundation of Sichuan University [2017SCU04A08]
  3. 2017 National Undergraduate Training Programs for Innovation and Entrepreneurship [201710616033]

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Nickel-rich layered oxides are regarded as very promising materials as cathodes for lithium-ion batteries because of their environmental benignancy, low cost, and high energy density. However, insufficient cycle performance and poor thermotic characteristics induced by structural degradation at high potentials and elevated temperatures pose challenging hurdles for nickel-rich cathodes. Here, a protective pillaring layer, in which partial Ni2+ ions occupy Li slabs induced by gradient Mn4+, is integrated into the primary particle of LiNi0.815Co0.15Al0.05O2 to stabilize the surface/interfacial structure. With the stable outer surface provided by the enriched Mn4+ gradient concentration and the pillar effect of the NiO-like phase, Mn-incorporated quaternary cathodes show enhanced structural stability and improved Li+ diffusion as well as lithium-storage properties. Compared with the severe capacity fade of a pure layered structure, the cathode with gradient Mn4+ exhibits more stable cycling behavior with a capacity retention of 80.0% after 500 cycles at 5.0 C.

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