Title: Enabling high energy lithium metal batteries via single-crystal Ni-rich cathode material co-doping strategy

Abstract

High-capacity Ni-rich layered oxides are promising cathode materials for secondary lithium-based battery systems. However, their structural instability detrimentally affects the battery performance during cell cycling. Here, we report an Al/Zr co-doped single-crystalline LiNi<:sub>0.88Co_0.09Mn_0.03O₂ (SNCM) cathode material to circumvent the instability issue. We found that soluble Al ions are adequately incorporated in the SNCM lattice while the less soluble Zr ions are prone to aggregate in the outer SNCM surface layer. The synergistic effect of Al/Zr co-doping in SNCM lattice improve the Li-ion mobility, relief the internal strain, and suppress the Li/Ni cation mixing upon cycling at high cut-off voltage. These features improve the cathode rate capability and structural stabilization during prolonged cell cycling. In particular, the Zr-rich surface enables the formation of stable cathode-electrolyte interphase, which prevent SNCM from unwanted reactions with the non-aqueous fluorinated liquid electrolyte solution and avoid Ni dissolution. To prove the practical application of the Al/Zr co-doped SNCM, we assembled a 10.8 Ah pouch cell (using a 100 μm thick Li metal anode) capable of delivering initial specific energy of 504.5 Wh kg-¹ at 0.1 °C and 25 °C.

Authors:

Ou, Xing  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-6302-7372"

Liu, Tongchao ^[2]; Zhong, Wentao ^[3]; Fan, Xinming ^[4]; Guo, Xueyi ^[4]; Huang, Xiaojing ^[5]; Cao, Liang ^[1]; Hu, Junhua  ^[6];

• Search DOE PAGES for author "Hu, Junhua"
• Search DOE PAGES for ORCID "0000-0003-0191-1503"

Zhang, Bao ^[4]; Chu, Yong S. ^[5]; Hu, Guorong ^[4]; Lin, Zhang ^[4]; Dahbi, Mouad ^[7]; Alami, Jones ^[7]; Amine, Khalil  ^[2];

• Search DOE PAGES for author "Amine, Khalil"
• Search DOE PAGES for ORCID "0000-0001-9206-3719"

Yang, Chenghao  ^[3];

• Search DOE PAGES for author "Yang, Chenghao"
• Search DOE PAGES for ORCID "0000-0002-3214-328X"

Lu, Jun  ^[2]

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• Search DOE PAGES for ORCID "0000-0003-0858-8577"

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+ Show Author Affiliations

1. South China Univ. of Technology (SCUT), Guangzhou (China); Central South University, Changsha (China)
2. Argonne National Lab. (ANL), Argonne, IL (United States)
3. South China Univ. of Technology (SCUT), Guangzhou (China)
4. Central South University, Changsha (China)
5. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
6. Zhengzhou University (China)
7. Mohammed VI Polytechnic University, Ben Guerir (Morocco)

Publication Date:

Thu Apr 28 00:00:00 EDT 2022

Research Org.:

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

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; Clean Vehicles, US-China Clean Energy Research Centre (CERC-CVC2)

OSTI Identifier:

1968743

Alternate Identifier(s):

OSTI ID: 1887536

Report Number(s):

BNL-223300-2022-JAAM
Journal ID: ISSN 2041-1723; 177586

Grant/Contract Number:  

AC02-06CH11357; SC0012704; 51922042; 51902347; 51872098

Resource Type:

Accepted Manuscript

Journal Name:

Nature Communications

Additional Journal Information:

Journal Volume: 13; Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:

Nature Publishing Group

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; 25 ENERGY STORAGE; Batteries; Inorganic chemistry; Transmission electron microscopy