Aggregate-Dominated Dilute Electrolytes with Low-Temperature-Resistant Ion-Conducting Channels for Highly Reversible Na Plating/Stripping

Ge, Bingcheng1; Deng, Jiaojiao2; Wang, Zhijie3; Liang, Qinghua4; Hu, Liang1; Ren, Xiuyun1; Li, Runmin5; Lin, Yuxiao5; Li, Yunsong6; Wang, Qingrong7; Han, Bin7; Deng, Yonghong7; Fan, Xiulin8; Li, Baohua9; Chen, Guohua10; Yu, Xiaoliang1

2024-08-01

10.1002/adma.202408161

ADVANCED MATERIALS   影响因子和分区

0935-9648

1521-4095

["Developing rechargeable batteries with high power delivery at low temperatures (LT) below 0 degrees C is significant for cold-climate applications. Initial anode-free sodium metal batteries (AFSMBs) promise high LT performances because of the low de-solvation energy and smaller Stokes radius of Na+, nondiffusion-limited plating/stripping electrochemistry, and maximized energy density. However, the severe reduction in electrolyte ionic conductivity and formation of unstable solid electrolyte interphase (SEI) hinder their practical applications at LT. In this study, a 2-methyltetrahydrofuran-based dilute electrolyte is designed to concurrently achieve an anion-coordinated solvation structure and impressive ionic conductivity of 3.58 mS cm-1 at -40 degrees C. The dominant aggregate solvates enable the formation of highly efficient and LT-resistant Na+ hopping channels in the electrolyte. Moreover, the methyl-regulated electronic structure in 2-methyltetrahydrofuran induces gradient decomposition toward an inorganic-organic bilayer SEI with high Na+ mobility, composition homogeneity, and mechanical robustness. As such, a record-high Coulombic efficiency beyond 99.9% is achieved even at -40 degrees C. The as-constructed AFSMBs sustain 300 cycles with 80% capacity maintained, and a 0.5-Ah level pouch cell delivers 85% capacity over 180 cycles at -25 degrees C. This study affords new insights into electrolyte formulation for fast ionic conduction and superior Na reversibility at ultralow temperatures.","A 2-methyltetrahydrofuran-based electrolyte is designed with weak dissociation of Na+-PF6- ion pairs and a highly efficient network for ultrafast Na+ hopping, which breaks through the LT ion-conducting limitation of conventional electrolytes. The methyl-regulated electronic structure induces gradient decomposition toward an inorganic-organic bilayer SEI with high Na+ mobility. A record-high CE beyond 99.9% is achieved even at -40 degrees C. image"]

anode free dilute electrolyte ion-conducting channel low temperature sodium metal battery

SCI ; EI

英语

其他

National Natural Science Foundation of China["52261160384","52072208"] ; Natural Science Foundation of Guangdong[2023A1515010020] ; Innovation and Technology Fund[ITS-325-22FP] ; Shenzhen Science and Technology Program[KJZD20230923114107014] ; Guangdong Basic and Applied Basic Research Foundation[2020A1515110798] ; Natural Science Fund for Colleges and Universities in Jiangsu Province[22KJB430004] ; Natural Science Foundation of Jiangxi[20232ACB214001]

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

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

WOS:001289284600001

WILEY-V C H VERLAG GMBH

MATERIALS SCIENCE

Web of Science

1.Hong Kong Polytech Univ, Dept Mech Engn, Hong Kong 999077, Peoples R China
2.Shenzhen Univ, Coll Chem & Environm Engn, Graphene Composite Res Ctr, Shenzhen 518060, Peoples R China
3.Hong Kong Polytech Univ, Dept Appl Phys, Hong Kong 999077, Peoples R China
4.Chinese Acad Sci, Ganjiang Innovat Acad, Key Lab Rare Earth, Ganzhou 341000, Jiangxi, Peoples R China
5.Jiangsu Normal Univ, Sch Phys & Elect Engn, Xuzhou 221116, Peoples R China
6.Zhejiang Lab, Hangzhou 311100, Peoples R China
7.Southern Univ Sci & Technol, Sch Innovat & Entrepreneurship, Dept Mat Sci & Engn, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China
8.Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon & Adv Semicond Mat, Hangzhou, Peoples R China
9.Tsinghua Univ, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Peoples R China
10.City Univ Hong Kong, Sch Energy & Environm, Hong Kong, Peoples R China

Ge, Bingcheng,Deng, Jiaojiao,Wang, Zhijie,et al. Aggregate-Dominated Dilute Electrolytes with Low-Temperature-Resistant Ion-Conducting Channels for Highly Reversible Na Plating/Stripping[J]. ADVANCED MATERIALS,2024.

Ge, Bingcheng.,Deng, Jiaojiao.,Wang, Zhijie.,Liang, Qinghua.,Hu, Liang.,...&Yu, Xiaoliang.(2024).Aggregate-Dominated Dilute Electrolytes with Low-Temperature-Resistant Ion-Conducting Channels for Highly Reversible Na Plating/Stripping.ADVANCED MATERIALS.

Ge, Bingcheng,et al."Aggregate-Dominated Dilute Electrolytes with Low-Temperature-Resistant Ion-Conducting Channels for Highly Reversible Na Plating/Stripping".ADVANCED MATERIALS (2024).