From Coating to Dopant: How the Transition Metal Composition Affects Alumina Coatings on Ni-Rich Cathodes

Han, Binghong; Key, Baris; Lapidus, Saul H.; Garcia, Juan C.; Iddir, Haim; Vaughey, John T.; Dogan, Fulya

doi:10.1021/acsami.7b13597

Title: From Coating to Dopant: How the Transition Metal Composition Affects Alumina Coatings on Ni-Rich Cathodes

Journal Article · Wed Nov 01 00:00:00 EDT 2017 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.7b13597· OSTI ID:1417024

^[1]; Key, Baris ^[1]; Lapidus, Saul H. ^[2];

^[3]; Iddir, Haim ^[3];

^[1];

^[1]

Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Sciences Division
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

Surface alumina coatings have been shown to be an effective way to improve the stability and cyclability of cathode materials. However, a detailed understanding of the relationship between the surface coatings and the bulk layered oxides is needed to better define the critical cathode–electrolyte interface. In this work, we systematically studied the effect of the composition of Ni-rich LiNi_xMn_yCo_1–x–yO₂ (NMC) on the surface alumina coatings. Changing cathode composition from LiNi_0.5Mn_0.3Co_0.2O₂ (NMC532) to LiNi_0.6Mn_0.2Co_0.2O₂ (NMC622) and LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) was found to facilitate the diffusion of surface alumina into the bulk after high-temperature annealing. By use of a variety of spectroscopic techniques, Al was seen to have a high bulk compatibility with higher Ni/Co content, and low bulk compatibility was associated with Mn in the transition metal layer. It was also noted that the cathode composition affected the observed morphology and surface chemistry of the coated material, which has an effect on electrochemical cycling. The presence of a high surface Li concentration and strong alumina diffusion into the bulk led to a smoother surface coating on NMC811 with no excess alumina aggregated on the surface. Structural characterization of pristine NMC particles also suggests surface Co segregation, which may act to mediate the diffusion of the Al from the surface to the bulk. The diffusion of Al into the bulk was found to be detrimental to the protection function of surface coatings leading to poor overall cyclability, indicating the importance of compatibility between surface coatings and bulk oxides on the electrochemical performance of coated cathode materials.In conclusion, these results are important in developing a better coating method for synthesis of next-generation cathode materials for lithium-ion batteries.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1417024

Journal Information:: ACS Applied Materials and Interfaces, Vol. 9, Issue 47; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 84 works

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36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
MAS NMR
NMC
TEM
alumina coating
aluminum doping
aluminum insertion
cathode materials
compositional effect

Title: From Coating to Dopant: How the Transition Metal Composition Affects Alumina Coatings on Ni-Rich Cathodes

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