Citation: LI Ya-Dong, DENG Yu-Feng, PAN Zhi-Yi, WEI Yin-Ping, ZHAO Shi-Xi, GAN Lin. Dual Electron Energy Loss Spectrum Imaging of the Surfaces of LiNi_0.5Mn_1.5O₄ Cathode Material[J]. Acta Physico-Chimica Sinica, ;2017, 33(11): 2293-2300. doi: 10.3866/PKU.WHXB201705294 shu

Dual Electron Energy Loss Spectrum Imaging of the Surfaces of LiNi_0.5Mn_1.5O₄ Cathode Material

LI Ya-Dong ^1,2, ,
DENG Yu-Feng ¹ ,
PAN Zhi-Yi ^1,2 ,
WEI Yin-Ping ^1,2 ,
ZHAO Shi-Xi ¹ ,
GAN Lin ^1,2

1.
Department of Energy and Environment, Graduate School at Shenzhen, Tsinghua University, Shenzhen 518055, Guangdong Province, P. R. China;
2.
Electron Microscopy Laboratory, Materials and Devices Testing Center, Graduate School at Shenzhen, Tsinghua University, Shenzhen 518055, Guangdong Province, P. R. China

Received Date: 24 April 2017
Revised Date: 19 May 2017

Fund Project: The project was supported by the Guangdong Natural Science Foundation for Distinguished Young Scholars, China (2016A030306035) and Shenzhen Basic Research Program, China (JCYJ20160531194754308).

Acquiring the spatial distribution of Li and the valence state of transition metals (TMs) in lithium ion battery (LIB) electrode materials is critical for understanding their electrochemical performances. Electron energy loss spectrum (EELS) is in principle optimum for analyzing light elements; however, quantitative analysis of Li, the lightest solid element in the periodic table, using EELS remains challenging. This is not only because of the overlap of the Li-K edge and the M₂₃ edge of TMs but also due to the normally large particle sizes of LIB electrode materials (hundreds of nm), leading to significant plural scattering effect in the EELS spectra. Using LiNi_0.5Mn_1.5O₄ (LNMO) as the cathode material, we obtained the spatial distribution of Li, Ni, and Mn by dual EELS spectral imaging, which allows us to simultaneously acquire the zero loss and core loss spectra, thus eliminating both the energy drift and plural scattering effects. Our results reveal that the as-prepared LNMO particles have a Mn/Ni-enriched and Li-poor surface layer of thickness 1-2 nm, and the valence of Mn gradually changed from +4 in the bulk to +2 in the surface layer. Given that the low-valent Mn²⁺ dissolution is a critical reason for structure damage and capacity degradation of LNMO, our results indicate that rational synthesis of LNMO with decreased low-valent Mn²⁺ content could be a previously neglected approach to enhance their electrochemical performance.
- Lithium ion battery,
- Li mapping,
- Valence state distribution,
- Electron energy loss spectroscopy,
- Spectrum imaging
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沈阳化工大学材料科学与工程学院沈阳 110142

Dual Electron Energy Loss Spectrum Imaging of the Surfaces of LiNi0.5Mn1.5O4 Cathode Material

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Dual Electron Energy Loss Spectrum Imaging of the Surfaces of LiNi_0.5Mn_1.5O₄ Cathode Material