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Title: Mn versus Al in Layered Oxide Cathodes in Lithium-Ion Batteries: A Comprehensive Evaluation on Long-Term Cyclability

Authors:
 [1];  [2];  [1];  [3];  [1];  [2]; ORCiD logo [1]
  1. Materials Science and Engineering Program and Texas Materials Institute, The University of Texas at Austin, Austin TX 78712 USA
  2. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge TN 37831 USA
  3. Bureau of Economic Geology, Jackson School of Geosciences, The University of Texas at Austin, Austin TX 78713 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1419355
Grant/Contract Number:
EE0007762
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Related Information: CHORUS Timestamp: 2018-02-02 02:23:19; Journal ID: ISSN 1614-6832
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Li, Wangda, Liu, Xiaoming, Celio, Hugo, Smith, Patrick, Dolocan, Andrei, Chi, Miaofang, and Manthiram, Arumugam. Mn versus Al in Layered Oxide Cathodes in Lithium-Ion Batteries: A Comprehensive Evaluation on Long-Term Cyclability. Germany: N. p., 2018. Web. doi:10.1002/aenm.201703154.
Li, Wangda, Liu, Xiaoming, Celio, Hugo, Smith, Patrick, Dolocan, Andrei, Chi, Miaofang, & Manthiram, Arumugam. Mn versus Al in Layered Oxide Cathodes in Lithium-Ion Batteries: A Comprehensive Evaluation on Long-Term Cyclability. Germany. doi:10.1002/aenm.201703154.
Li, Wangda, Liu, Xiaoming, Celio, Hugo, Smith, Patrick, Dolocan, Andrei, Chi, Miaofang, and Manthiram, Arumugam. 2018. "Mn versus Al in Layered Oxide Cathodes in Lithium-Ion Batteries: A Comprehensive Evaluation on Long-Term Cyclability". Germany. doi:10.1002/aenm.201703154.
@article{osti_1419355,
title = {Mn versus Al in Layered Oxide Cathodes in Lithium-Ion Batteries: A Comprehensive Evaluation on Long-Term Cyclability},
author = {Li, Wangda and Liu, Xiaoming and Celio, Hugo and Smith, Patrick and Dolocan, Andrei and Chi, Miaofang and Manthiram, Arumugam},
abstractNote = {},
doi = {10.1002/aenm.201703154},
journal = {Advanced Energy Materials},
number = ,
volume = ,
place = {Germany},
year = 2018,
month = 2
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on February 2, 2019
Publisher's Accepted Manuscript

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  • The Ni-rich layered oxides with a Ni content of >0.5 are drawing much attention recently to increase the energy density of lithium-ion batteries. However, the Ni-rich layered oxides suffer from aggressive reaction of the cathode surface with the organic electrolyte at the higher operating voltages, resulting in consequent impedance rise and capacity fade. To overcome this difficulty, we present here a heterostructure composed of a Ni-rich LiNi 0.7Co 0.15Mn 0.15O 2 core and a Li-rich Li 1.2-xNi 0.2Mn 0.6O 2 shell, incorporating the advantageous features of the structural stability of the core and chemical stability of the shell. With amore » unique chemical treatment for the activation of the Li 2MnO 3 phase of the shell, a high capacity is realized with the Li-rich shell material. Aberration-corrected scanning transmission electron microscopy (STEM) provides direct evidence for the formation of surface Li-rich shell layer. Finally, the heterostructure exhibits a high capacity retention of 98% and a discharge- voltage retention of 97% during 100 cycles with a discharge capacity of 190 mA h g -1 (at 2.0–4.5 V under C/3 rate, 1C = 200 mA g -1).« less
  • Lattice oxygen can play an intriguing role in electrochemical processes, not only maintaining structural stability, but also influencing electron and ion transport properties in high-capacity oxide cathode materials for Li-ion batteries. Here, we report the design of a gas–solid interface reaction to achieve delicate control of oxygen activity through uniformly creating oxygen vacancies without affecting structural integrity of Li-rich layered oxides. Theoretical calculations and experimental characterizations demonstrate that oxygen vacancies provide a favourable ionic diffusion environment in the bulk and significantly suppress gas release from the surface. The target material is achievable in delivering a discharge capacity as high asmore » 301 mAh g –1 with initial Coulombic efficiency of 93.2%. After 100 cycles, a reversible capacity of 300 mAh g –1 still remains without any obvious decay in voltage. Lastly, this study sheds light on the comprehensive design and control of oxygen activity in transition-metal-oxide systems for next-generation Li-ion batteries.« less
  • Lattice oxygen can play an intriguing role in electrochemical processes, not only maintaining structural stability, but also influencing electron and ion transport properties in high-capacity oxide cathode materials for Li-ion batteries. We report the design of a gas–solid interface reaction to achieve delicate control of oxygen activity through uniformly creating oxygen vacancies without affecting structural integrity of Li-rich layered oxides. Furthermore, theoretical calculations and experimental characterizations demonstrate that oxygen vacancies provide a favourable ionic diffusion environment in the bulk and significantly suppress gas release from the surface. The target material is achievable in delivering a discharge capacity as high asmore » 301 mAh g -1 with initial Coulombic efficiency of 93.2%. After 100 cycles, a reversible capacity of 300 mAh g -1 still remains without any obvious decay in voltage. Our study sheds light on the comprehensive design and control of oxygen activity in transition-metal-oxide systems for next-generation Li-ion batteries.« less