In Situ Probing and Synthetic Control of Cationic Ordering in Ni-Rich Layered Oxide Cathodes
Abstract
Ni-rich layered oxides (LiNi1-xMxO2; 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 LiNi1-xMxO2 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, LiNi0.8Co0.2O2, 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 LiNi0.8Co0.2O2 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.
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1768777
- Alternate Identifier(s):
- OSTI ID: 1389223; OSTI ID: 1401242
- Report Number(s):
- BNL-221104-2021-JAAM; BNL-114130-2017-JA
Journal ID: ISSN 1614-6832
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 3; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 25 ENERGY STORAGE
Citation Formats
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, and Wang, Feng. In Situ Probing and Synthetic Control of Cationic Ordering in Ni-Rich Layered Oxide Cathodes. United States: N. p., 2016.
Web. doi:10.1002/aenm.201601266.
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. In Situ Probing and Synthetic Control of Cationic Ordering in Ni-Rich Layered Oxide Cathodes. United States. https://doi.org/10.1002/aenm.201601266
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, and Wang, Feng. Mon .
"In Situ Probing and Synthetic Control of Cationic Ordering in Ni-Rich Layered Oxide Cathodes". United States. https://doi.org/10.1002/aenm.201601266. https://www.osti.gov/servlets/purl/1768777.
@article{osti_1768777,
title = {In Situ Probing and Synthetic Control of Cationic Ordering in Ni-Rich Layered Oxide Cathodes},
author = {Zhao, Jianqing and Zhang, Wei and Huq, Ashfia and Misture, Scott T. and Zhang, Boliang and Guo, Shengmin and Wu, Lijun and Zhu, Yimei and Chen, Zonghai and Amine, Khalil and Pan, Feng and Bai, Jianming and Wang, Feng},
abstractNote = {Ni-rich layered oxides (LiNi1-xMxO2; 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 LiNi1-xMxO2 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, LiNi0.8Co0.2O2, 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 LiNi0.8Co0.2O2 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.},
doi = {10.1002/aenm.201601266},
journal = {Advanced Energy Materials},
number = 3,
volume = 7,
place = {United States},
year = {Mon Oct 17 00:00:00 EDT 2016},
month = {Mon Oct 17 00:00:00 EDT 2016}
}
Web of Science
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