Constructing Uniform and Robust Li<sub>3</sub>N Interface by Methacrylamide Additive Achieves High Performance of LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> Battery

Because the traditional electrolyte is unstable at high voltage, the commercial use of LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> in power batteries still faces huge challenges. Regarding this, the introduction of additives directly into the electrolyte is one of the easiest ways. Herein, an amide compound, methacrylamide (MAA), is proposed as a novel additive into the conventional electrolyte in our work. The amino group (-NH<sub>2</sub>) in MAA can undergo coordination and complexation reaction with strong lewis acid PF<sub>5</sub>. Additionally, MAA can be preferentially oxidized to stabilize the electrolyte and decomposed to generate nitrogen-containing (Li<sub>3</sub>N) interface components with high ionic conductivity. Therefore, the Li/LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> battery with 0.5 wt % MAA electrolyte delivers an initial specific discharge capacity of 141.7 mAh·g<sup>-1</sup> and maintaining an outstanding capacity retention rate (95.2%) and a very high average Coulombic efficiency (99.1%) after 200 cycles at 0.2C. MAA provides a new idea for broadening the application of carbonate electrolytes under a high voltage.

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Publication Details

Journal
The Journal of Physical Chemistry Letters
Published
2025-06-16
DOI
https://doi.org/10.1021/acs.jpclett.5c01042
Citations
1
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
0.73

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article en
1 citations

Abstract

Because the traditional electrolyte is unstable at high voltage, the commercial use of LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> in power batteries still faces huge challenges. Regarding this, the introduction of additives directly into the electrolyte is one of the easiest ways. Herein, an amide compound, methacrylamide (MAA), is proposed as a novel additive into the conventional electrolyte in our work. The amino group (-NH<sub>2</sub>) in MAA can undergo coordination and complexation reaction with strong lewis acid PF<sub>5</sub>. Additionally, MAA can be preferentially oxidized to stabilize the electrolyte and decomposed to generate nitrogen-containing (Li<sub>3</sub>N) interface components with high ionic conductivity. Therefore, the Li/LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> battery with 0.5 wt % MAA electrolyte delivers an initial specific discharge capacity of 141.7 mAh·g<sup>-1</sup> and maintaining an outstanding capacity retention rate (95.2%) and a very high average Coulombic efficiency (99.1%) after 200 cycles at 0.2C. MAA provides a new idea for broadening the application of carbonate electrolytes under a high voltage.

The Journal of Physical Chemistry LettersVol. 16(25)
Suzhou Research Institute (CN), Hubei University (CN)
National Natural Science Foundation of China
Openalex Percentile: Top 27%
Advancements in Battery Materials
0.73
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Constructing Uniform and Robust Li<sub>3</sub>N Interface by Methacrylamide Additive Achieves High Performance of LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> Battery — Tianxiang Ren, Siqi Zhong, et al. · The Journal of Physical Chemistry Letters (2025) | TGRS Research Map | TGRS