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Research Article

Boosting the energy density of sulfide-based all-solid-state batteries at low temperatures by charging to high voltages up to 6 V

Lun Zhang1,§, Xuedong Zhang1,§, Zhaoyu Rong2, Tao Wang2, Zhenyu Wang3( ), Zaifa Wang2,4, Longchen Zhang5, Qiao Huang1, Lingyun Zhu6, Liqiang Zhang2( ), Yongfu Tang2,5( ), Jianyu Huang1,2( )
Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education, School of Materials Science and Engineering, Xiangtan University, Xiangtan 411105, China
Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, China
Guilin Electrical Equipment Scientific Research Institute Co., Ltd, Guilin 541004, China
GRINM (Guangdong) Institute for Advanced Materials and Technology, Foshan 528000, China
Hebei Key Laboratory of Applied Chemistry, College of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao 066004, China
School of Materials Science & Engineering, Anhui University, Hefei 230601, China

§ Lun Zhang and Xuedong Zhang contributed equally to this work.

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Graphical Abstract

The energy density of all-solid-state batteries (ASSBs) at low temperatures can be improved dramatically by reducing the solid electrolyte thickness and charging to high voltages up to 6 V without damaging the LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode materials, which differs considerably from the room temperature ASSBs.

Abstract

Sulfide electrolyte-based all-solid-state batteries (ASSBs) are potential next generation energy storage technology due to the high ionic conductivity of sulfide electrolytes and potentially improved energy density and safety. However, the performance of ASSBs at/below subzero temperatures has not been explored systematically. Herein, low temperature (LT) performance of LiNi0.8Co0.1Mn0.1O2 (NCM811)|Li9.54Si1.74P1.44S11.7Cl0.3 (LiSPSCl)|Li4Ti5O12 (LTO) ASSBs was investigated. By charging the ASSB to 6 V at −40 °C, a capacity of 100.7 mAh∙g−1 at 20 mA∙g−1 was achieved, which is much higher than that charged to 4.3 V (4.6 mAh∙g−1) at −40 °C. Moreover, atomic resolution microscopy revealed that the NCM811 remained almost intact even after being charged to 6 V. In contrast, NCM811 was entirely destructed when charged to 6 V at room temperature. The sharp difference arises from the large internal charge transfer resistance at LT which requires high voltage to overcome. Nevertheless, such high voltage is not harmful to the active material but beneficial to extracting most energy out of the ASSBs at LT. We also demonstrated that thinner electrolyte is favorable for LT operation of ASSBs due to the reduced ion transfer distance. This work provides new strategies to boost the capacity and energy density of sulfide-based ASSBs at LT for dedicated LT applications.

Keywords

all-solid-state lithium batteriessulfide solid electrolytelow temperatureLi4Ti5O12 (LTO)

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Nano Research
Volume 16 Issue 8,
August 2023
Pages 10966-10975
DOI: 10.1007/s12274-023-5827-3
Cite this article:
Zhang L, Zhang X, Rong Z, et al. Boosting the energy density of sulfide-based all-solid-state batteries at low temperatures by charging to high voltages up to 6 V. Nano Research, 2023, 16(8): 10966-10975. https://doi.org/10.1007/s12274-023-5827-3
Topics:
Lithium batteries

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Received: 15 March 2023
Revised: 09 May 2023
Accepted: 10 May 2023
Published: 13 June 2023
© Tsinghua University Press 2023
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