Suppressed Internal Intrinsic Stress Engineering in High-Performance Ni-Rich Cathode Via Multilayered In Situ Coating Structure

Jiachao Yang; Yunjiao Li; Xiaoming Xi; Junchao Zheng; Jian Yu; Zhenjiang He

doi:10.1002/eem2.12574

Energy & Environmental Materials ›› 2024, Vol. 7 ›› Issue (2) :12574 DOI: 10.1002/eem2.12574

RESEARCH ARTICLE

Suppressed Internal Intrinsic Stress Engineering in High-Performance Ni-Rich Cathode Via Multilayered In Situ Coating Structure

Jiachao Yang ¹^,²
, Yunjiao Li ¹^,²^,^†
, Xiaoming Xi ³
, Junchao Zheng ¹^,²
, Jian Yu ⁴
, Zhenjiang He ¹^,²

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Abstract

LiNi_xCo_yAl_zO₂(NCA) cathode materials are drawing widespread attention, but the huge gap between the ideal and present cyclic stability still hinders their further commercial application, especially for the Ni-rich LiNi_xCo_yAl_zO₂ (x > 0.8, x + y + z = 1) cathode material, which is owing to the structural degradation and particles' intrinsic fracture. To tackle the problems, Li_0.5La₂Al_0.5O₄ in situ coated and Mn compensating doped multilayer LiNi_0.82Co_0.14Al_0.04O₂ was prepared. XRD refinement indicates that La-Mn co-modifying could realize appropriate Li/Ni disorder degree. Calculated results and in situ XRD patterns reveal that the LLAO coating layer could effectively restrain crack in secondary particles benefited from the suppressed internal strain. AFM further improves as NCA-LM2 has superior mechanical property. The SEM, TEM, XPS tests indicate that the cycled cathode with LLAO-Mn modification displays a more complete morphology and less side reaction with electrolyte. DEMS was used to further investigate cathode-electrolyte interface which was reflected by gas evolution. NCA-LM2 releases less CO₂ than NCA-P indexing on a more stable surface. The modified material presents outstanding capacity retention of 96.2% after 100 cycles in the voltage range of 3.0-4.4 V at 1C, 13% higher than that of the pristine and 80.8% at 1 C after 300 cycles. This excellent electrochemical performance could be attributed to the fact that the high chemically stable coating layer of Li_0.5La₂Al_0.5O₄ (LLAO) could enhance the interface and the Mn doping layer could suppress the influence of the lattice mismatch and distortion. We believe that it can be a useful strategy for the modification of Ni-rich cathode material and other advanced functional material.

Keywords

compensating doped / in situ coating / multilayer material / Ni-rich cathode materials / suppressed internal strain

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Jiachao Yang, Yunjiao Li, Xiaoming Xi, Junchao Zheng, Jian Yu, Zhenjiang He. Suppressed Internal Intrinsic Stress Engineering in High-Performance Ni-Rich Cathode Via Multilayered In Situ Coating Structure. Energy & Environmental Materials, 2024, 7(2): 12574 DOI:10.1002/eem2.12574

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