Superior Li+ Kinetics by "Low-Activity-Solvent" Engineering for Stable Lithium Metal Batteries

Haifeng Tu; Zhigang He; Ao Sun; Farwa Mushtaq; Linge Li; Zhicheng Wang; Yaping Kong; Rong Huang; Hongzhen Lin; Wanfei Li; Fangmin Ye; Pan Xue; Meinan Liu

doi:10.1021/acs.nanolett.4c00501

Superior Li⁺ Kinetics by "Low-Activity-Solvent" Engineering for Stable Lithium Metal Batteries

Nano Lett. 2024 May 15;24(19):5714-5721. doi: 10.1021/acs.nanolett.4c00501. Epub 2024 May 2.

Authors

Haifeng Tu^{1

2}, Zhigang He², Ao Sun², Farwa Mushtaq^{1

2}, Linge Li^{1

2}, Zhicheng Wang^{1

2}, Yaping Kong², Rong Huang², Hongzhen Lin^{1

2}, Wanfei Li³, Fangmin Ye⁴, Pan Xue⁵, Meinan Liu^{2

6

7

8}

Affiliations

¹ School of Nano-Tech and Nano-Bionics, University of Science and Technology of China, Hefei, Anhui 230026, China.
² Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, Jiangsu 215123, China.
³ Suzhou Key Laboratory for Nanophotonic and Nanoelectronic Materials and Its Devices, School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou, Jiangsu 215009, China.
⁴ Center for Optoelectronic Materials and Devices, Key Laboratory of Optical Field Manipulation of Zhejiang Province, Zhejiang Sci-Tech University, Hangzhou 310018, China.
⁵ School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, China.
⁶ State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, School of Resources, Environment and Materials, Guangxi University, Nanning 530004, China.
⁷ Guangdong Institute of Semiconductor Micro-nano Manufacturing Technology, Foshan 528225, China.
⁸ Division of Nanomaterials and Jiangxi Key Lab of Carbonene Materials, Jiangxi Institute of Nanotechnology, Nanchang 330200, China.

PMID: 38695488
DOI: 10.1021/acs.nanolett.4c00501

Abstract

The structure of solvated Li⁺ has a significant influence on the electrolyte/electrode interphase (EEI) components and desolvation energy barrier, which are two key factors in determining the Li⁺ diffusion kinetics in lithium metal batteries. Herein, the "solvent activity" concept is proposed to quantitatively describe the correlation between the electrolyte elements and the structure of solvated Li⁺. Through fitting the correlation of the electrode potential and solvent concentration, we suggest a "low-activity-solvent" electrolyte (LASE) system for deriving a stable inorganic-rich EEI. Nano LiF particles, as a model, were used to capture free solvent molecules for the formation of a LASE system. This advanced LASE not only exhibits outstanding antidendrite growth behavior but also delivers an impressive performance in Li/LiNi_0.8Co_0.1Mn_0.1O₂ cells (a capacity of 169 mAh g^-1 after 250 cycles at 0.5 C).

Keywords: desolvation; electrolyte/electrode interphase; lithium metal batteries; solvation structure; “low-activity-solvent” electrolyte.