Title: Evolution of redox couples in Li- and Mn-rich cathode materials and mitigation of voltage fade by reducing oxygen release

Abstract

Here, voltage fade is a major problem in battery applications for high-energy Lithium- and Manganese-rich (LMR) layered materials. Because of the complexity in the LMR structure, the voltage fade mechanism is not well understood. Here we conduct in situ and ex situ studies on a typical LMR material (Li_1.2Ni_0.15Co_0.1Mn_0.55O₂) during charge-discharge cycling, using multi-length-scale X-ray spectroscopic and 3D electron microscopic imaging techniques. Through probing from surface to bulk, from individual to the whole ensembles of particles, we show that the average valence states of each type of transition metal cations are continuously reduced, which is attributed to the oxygen release from LMR.

Authors:

Hu, Enyuan  ^[1];

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Yu, Xiqian  ^[2];

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Lin, Ruoqian ^[3]; Bi, Xuanxuan ^[4]; Lu, Jun  ^[4];

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Bak, Seongmin ^[1]; Nam, Kyung-Wan  ^[5];

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Xin, Huolin L.  ^[6];

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Jaye, Cherno ^[7]; Fischer, Daniel A. ^[7]; Amine, Kahlil ^[4]; Yang, Xiao-Qing ^[1]

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+ Show Author Affiliations

1. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division; Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics and Inst. of Physics
3. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division and Center for Functional Nanomaterials (CFN)
4. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
5. Dongguk Univ., Seoul (Korea, Republic of). Dept. of Energy and Materials Engineering
6. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
7. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Material Measurement Lab.

Publication Date:

2018-07-30

Research Org.:

Argonne National Lab. (ANL), Argonne, IL (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Org.:

USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES); Chinese Academy of Sciences (CAS); National Key R&D Program of China; National Natural Science Foundation of China (NSFC); National Research Foundation of Korea (NRF)

OSTI Identifier:

1467843

Alternate Identifier(s):

OSTI ID: 1460715

Report Number(s):

BNL-207813-2018-JAAM
Journal ID: ISSN 2058-7546; 144252

Grant/Contract Number:  

AC02-06CH11357; SC0012704; 2016YFA0202500; 51421002; NRF-2017M1A2A2044502; AC02-98CH10886

Resource Type:

Accepted Manuscript

Journal Name:

Nature Energy

Additional Journal Information:

Journal Volume: 3; Journal Issue: 8; Journal ID: ISSN 2058-7546

Publisher:

Nature Publishing Group

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; 25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; batteries; electrochemistry