Regulating Electrolyte Solvation Structures via Diluent-Solvent Interactions for Safe High-Voltage Lithium Metal Batteries

Liu, Yuqi1; Li, Jin2; Deng, Xiaolan3; Chi, Shang-Sen4; Wang, Jun4; Zeng, Huipeng4; Jiang, Yidong1; Li, Tingting5; Liu, Zhongbo6; Wang, Hui1; Zhang, Guangzhao1,4,7; Deng, Yonghong4; Wang, Chaoyang1,7

2024-03-01

10.1002/smll.202311812

SMALL   影响因子和分区

1613-6810

1613-6829

Local high concentration electrolytes (LHCEs) have been proved to be one of the most promising systems to stabilize both high voltage cathodes and Li metal anode for next-generation batteries. However, the solvation structures and interactions among different species in LHCEs are still convoluted, which bottlenecks the further breakthrough on electrolyte development. Here, it is demonstrated that the hydrogen bonding interaction between diluent and solvent is crucial for the construction of LHCEs and corresponding interphase chemistries. The 2,2,2-trifluoroethyl trifluoromethane sulfonate (TFSF) is selected as diluent with the solvent dimethoxy-ethane (DME) to prepare a non-flammable LHCE for high voltage LMBs. This is first find that the hydrogen bonding interaction between TFSF and DME solvent tailors the electrolyte solvation structures by weakening the coordination of DME molecules to Li+ cations and allows more participation of anions in the first solvation shell, leading to the formation of aggregates (AGGs) clusters which are conducive to generating inorganic solid/cathodic electrolyte interphases (SEI/CEIs). The proposed TFSF based LHCE enables the Li||NCM811 (LiNi0.8Mn0.1O2) batteries to realize >80% capacity retention with a high average Coulombic efficiency of 99.8% for 230 cycles under aggressive conditions (NCM811 cathode: 3.4 mAh cm(-2), cut-off voltage: 4.4 V, and 20 mu m Li foil).

diluent-solvent interaction lithium metal battery local high concentration non-flammable solvation structure

SCI ; EI

英语

通讯

Science and Technology Planning Project of Guangdong Province[2021A0505110001] ; Opening Project of Key Laboratory of Polymer Processing Engineering[KFKT2302] ; Shenzhen Science and Technology Major Project[KJZD20230923114222046] ; null[22305115] ; null[22275059]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:001177513400001

WILEY-V C H VERLAG GMBH

20241015704949

Cathodes ; Electrolytes ; Hydrogen ; Hydrogen bonds ; Lithium ; Lithium batteries ; Nickel compounds ; Solvation

Lithium and Alloys:542.4 ; Alkali Metals:549.1 ; Electric Batteries and Fuel Cells:702 ; Primary Batteries:702.1.1 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804

Web of Science

1.South China Univ Technol, Res Inst Mat Sci, Guangzhou 510640, Peoples R China
2.GAC Aion New Energy Automobile Co Ltd, Res & Dev Ctr, Guangzhou 510640, Peoples R China
3.Zen Semicond Corp, Guangzhou 510000, Peoples R China
4.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
5.Keji Rd South,Hitech Ind Pk, Shenzhen 518057, Peoples R China
6.Shenzhen CAPCHEM Technol Co Ltd, Shenzhen 518118, Peoples R China
7.South China Univ Technol, Key Lab Polymer Proc Engn, Minist Educ, Guangzhou 510640, Peoples R China

Liu, Yuqi,Li, Jin,Deng, Xiaolan,et al. Regulating Electrolyte Solvation Structures via Diluent-Solvent Interactions for Safe High-Voltage Lithium Metal Batteries[J]. SMALL,2024,20.

Liu, Yuqi.,Li, Jin.,Deng, Xiaolan.,Chi, Shang-Sen.,Wang, Jun.,...&Wang, Chaoyang.(2024).Regulating Electrolyte Solvation Structures via Diluent-Solvent Interactions for Safe High-Voltage Lithium Metal Batteries.SMALL,20.

Liu, Yuqi,et al."Regulating Electrolyte Solvation Structures via Diluent-Solvent Interactions for Safe High-Voltage Lithium Metal Batteries".SMALL 20(2024).