Molecular Design of Competitive Solvation Electrolytes for Practical High-Energy and Long-Cycling Lithium-Metal Batteries

doi:10.1002/adfm.202312413

	Molecular Design of Competitive Solvation Electrolytes for Practical High-Energy and Long-Cycling Lithium-Metal Batteries
	Zhang, Guangzhao 1,2; Li, Jiawei 3; Chi, Shang-Sen 1; Wang, Jun 1; Wang, Qingrong 1; Ke, Ruohong 1; Liu, Zhongbo 4; Wang, Hui2 ; Wang, Chaoyang 2; Chang, Jian 1,5; Deng, Yonghong 1; Lu, Jun 6
	2023-12-21
发表期刊	ADVANCED FUNCTIONAL MATERIALS
ISSN	1616-301X
页码	11
通讯作者	Chang, Jian(changj@gbu.edu.cn) ; Deng, Yonghong(yhdeng08@163.com) ; Lu, Jun(junzoelu@zju.edu.cn)
摘要	Electrolytes with high stability against both Li anode and high-voltage cathode are critical for high-energy and long-cycling lithium metal batteries (LMBs). However, the free active solvents in common electrolytes are susceptible to decomposition at both Li anode and high-voltage cathode. Although recently developed locally high-concentration electrolytes (LHCEs) have largely restricted active solvents via Li+ coordination, the free molecules are still released upon the desolvation of Li+ at the surface of electrodes, causing continuous decomposition during long-cycling processes. Here, a molecule competitive solvation electrolyte (MCE) is shown to stabilize high-voltage LMBs by introducing a well-designed and newly synthetic bipolar solvent molecule with one ion-dissociative polar head and the other highly fluorinated nonpolar tail. The bipolar molecules competitively dissociate Li+ via weak coordination interactions, drastically reducing the ratio of active solvents in electrolytes and the detrimental decomposition at electrodes during the desolvation processes. Consequently, the MCE enables a 1.4-Ah Li metal pouch cell with a stack energy density of 450 Wh kg-1 along with exceptional operation stability over 400 cycles (retention: 81%). Furthermore, the MCE also maintains the stable operation of a 2.5-Ah Li-S pouch cell with an excellent energy density of 417 Wh kg-1 for 70 cycles under practical conditions. A competitive solvation electrolyte enabled by a well-designed bipolar molecule is proposed to reduce the detrimental decomposition of active solvents with Li anodes and high-voltage cathodes, thus enabling a 1.4-Ah high-voltage pouch cell with the energy density of 450 Wh kg-1 along with long cycling stability (retention: 81% after 400 cycles) under aggressive conditions.image
关键词	bipolar molecule competitive solvation electrolyte high voltage lithium metal batteries molecular design
DOI	10.1002/adfm.202312413
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China ; Guangdong Basic and Applied Basic Research Foundation[2022A1515011005] ; Guangdong Basic and Applied Basic Research Foundation[2023A1515010686] ; Shenzhen Science and Technology Program[JCYJ20220818100218040] ; Opening Project of Key Laboratory of Polymer Processing Engineering[KFKT2302] ; Science and Technology Planning Project of Guangdong Province[2021A0505110001] ; [22371116] ; [22305115] ; [22078144]
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS类目	Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号	WOS:001128492400001
出版者	WILEY-V C H VERLAG GMBH
WOS关键词	ION ; SOLVENTS
引用统计	被引频次：1[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.qdio.ac.cn/handle/337002/184204
专题	海洋环境腐蚀与生物污损重点实验室
通讯作者	Chang, Jian; Deng, Yonghong; Lu, Jun
作者单位	1.Southern Univ Sci & Technol, Key Univ Lab Highly Efficient Utilizat Solar Energ, Sch Innovat & Entrepreneurship, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China 2.South China Univ Technol, Res Inst Mat Sci, Key Lab Polymer Proc Engn, Guangzhou 510640, Peoples R China 3.Chinese Acad Sci, Inst Oceanol, Key Lab Marine Environm Corros & Biofouling, Qingdao 266071, Peoples R China 4.Shenzhen CAPCHEM Technol Co Ltd, Shenzhen 518118, Peoples R China 5.Great Bay Univ, Sch Phys Sci, Dongguan 523000, Guangdong, Peoples R China 6.Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310058, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Guangzhao,Li, Jiawei,Chi, Shang-Sen,et al. Molecular Design of Competitive Solvation Electrolytes for Practical High-Energy and Long-Cycling Lithium-Metal Batteries[J]. ADVANCED FUNCTIONAL MATERIALS,2023:11.
APA	Zhang, Guangzhao.,Li, Jiawei.,Chi, Shang-Sen.,Wang, Jun.,Wang, Qingrong.,...&Lu, Jun.(2023).Molecular Design of Competitive Solvation Electrolytes for Practical High-Energy and Long-Cycling Lithium-Metal Batteries.ADVANCED FUNCTIONAL MATERIALS,11.
MLA	Zhang, Guangzhao,et al."Molecular Design of Competitive Solvation Electrolytes for Practical High-Energy and Long-Cycling Lithium-Metal Batteries".ADVANCED FUNCTIONAL MATERIALS (2023):11.

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