In Situ Probing and Synthetic Control of Cationic Ordering in Ni-Rich Layered Oxide Cathodes

Zhao, Jianqing; Zhang, Wei; Huq, Ashfia; Misture, Scott T.; Zhang, Boliang; Guo, Shengmin; Wu, Lijun; Zhu, Yimei; Chen, Zonghai; Amine, Khalil; Pan, Feng; Bai, Jianming; Wang, Feng

doi:10.1002/aenm.201601266

Title: In Situ Probing and Synthetic Control of Cationic Ordering in Ni-Rich Layered Oxide Cathodes

Journal Article · Mon Oct 17 00:00:00 EDT 2016 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201601266· OSTI ID:1768777

Zhao, Jianqing ^[1]; Zhang, Wei ^[1]; Huq, Ashfia ^[2]; Misture, Scott T. ^[3]; Zhang, Boliang ^[4]; Guo, Shengmin ^[4]; Wu, Lijun ^[1]; Zhu, Yimei ^[1]; Chen, Zonghai ^[5]; Amine, Khalil ^[5]; Pan, Feng ^[6]; Bai, Jianming ^[1]; Wang, Feng ^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Alfred Univ., NY (United States)
Louisiana State Univ., Baton Rouge, LA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Peking Univ. Shenzhen Graduate School, Shenzhen (China)

Ni-rich layered oxides (LiNi_1-xM_xO₂; M=Co, Mn, …) are appealing alternatives to conventional LiCoO₂ as cathodes in Li-ion batteries for automobile and other large-scale applications due to their high theoretical capacity and low cost. However, preparing stoichiometric LiNi_1-xM_xO₂ with ordered layer structure and high reversible capacity, has proven difficult due to Ni²⁺/Li⁺ cation mixing in octahedral sites. Herein, we report on in-situ studies of synthesis reactions and the associated structural ordering in preparing LiNiO₂ and the Co-substituted variant, LiNi_0.8Co_0.2O₂, thereby gaining insights into synthetic control of the structure and electrochemical properties of Ni-rich layered oxides. Results from this study indicate a direct transformation of the intermediate from the rock salt structure into hexagonal phase, and during the process, Co substitution facilities the nucleation of a Co-rich layered phase at low temperatures and subsequent growth and stabilization of solid solution Li(Ni, Co)O₂ upon heat treatment in a highly oxidation environment. Optimal conditions were identified from the in-situ studies and utilized in obtaining stoichiometric LiNi_0.8Co_0.2O₂ that exhibits high capacity of about 200 mAh/g with excellent retention. The findings shed light on designing Ni-rich layered oxide cathodes with enhanced electrochemical properties through synthetic control of the structural ordering in the materials.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC0012704

OSTI ID:: 1768777

Alternate ID(s):: OSTI ID: 1389223; OSTI ID: 1401242

Report Number(s):: BNL-221104-2021-JAAM; BNL-114130-2017-JA

Journal Information:: Advanced Energy Materials, Vol. 7, Issue 3; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 188 works

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