High-Concentration Additive and Triiodide/Iodide Redox Couple Stabilize Lithium Metal Anode and Rejuvenate the Inactive Lithium in Carbonate-Based Electrolyte

Wen, Zuxin1; Fang, Wenqiang1; Wu, Xiaoyu2; Qin, Zuoyu1; Kang, Hong1; Chen, Long1; Zhang, Ning1; Liu, Xiaohe3; Chen, Gen1

2022-06-01

10.1002/adfm.202204768

ADVANCED FUNCTIONAL MATERIALS   影响因子和分区

1616-301X

1616-3028

Carbonate-based electrolytes are incompatible with lithium (Li) metal anode because the generated solid electrolyte interphase (SEI) undergoes repeated breakage-repair, resulting in the accumulation of inactive Li including Li+ compounds and electrically isolated dead Li-0 in the SEI. Therefore, exploiting a suitable strategy to construct a stable SEI while efficiently rejuvenating the inactive Li capacity is urgent and more thoughtful than just building a stereotyped SEI layer. Herein, an innovative strategy is proposed of high-concentration additive (HCA) of LiNO3 inspired by (localized) high-concentration electrolyte and inactive Li restoration methodology via triiodide/iodide (I-3(-)/I-) redox couple to improve the compatibility of carbonate-based electrolytes. The HCA of LiNO3 can maintain the cation-anion aggregates solvation structures in the carbonate-based bulk electrolyte and induce the in situ formation of superior-ionic-conductivity NO3--derived SEI. Moreover, the reversible I-3(-)/I- redox couple can further optimize the SEI and constantly rejuvenate the inactive Li including solvent/LiNO3-derived Li2O, a derivative has almost been acquiescent in LiNO3-additive electrolytes, and dead Li-0 into delithiated cathode. Consequently, epitaxy-like planar Li deposition, better reversibility, and higher capacity retention can be realized and are systematically verified by Li||Cu half cells, full cells with excess/limited Li (N/P ratio = 1.5) and anode-free lithium metal batteries.

high-concentration additives inactive Li rejuvenation lithium nitrate redox couples

SCI ; EI

英语

NI论文

其他

Natural Science Foundation for Distinguished Young Scholars of Hunan Province[2022JJ10089] ; National Natural Science Foundation of China[52002405,"U20A20123",51874357] ; "Huxiang high-level talents" program[2019RS1007]

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

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

WOS:000814184400001

WILEY-V C H VERLAG GMBH

20222512256455

Anodes ; Carbonation ; Lithium compounds ; Lithium-ion batteries ; Seebeck effect ; Solid electrolytes ; Solid-State Batteries

Electricity: Basic Concepts and Phenomena:701.1 ; Secondary Batteries:702.1.2 ; Electron Tubes:714.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803

MATERIALS SCIENCE

Web of Science

1.Cent South Univ, Sch Mat Sci & Engn, Changsha 410083, Hunan, Peoples R China
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
3.Zhengzhou Univ, Sch Chem Engn, Zhengzhou 450001, Henan, Peoples R China

Wen, Zuxin,Fang, Wenqiang,Wu, Xiaoyu,et al. High-Concentration Additive and Triiodide/Iodide Redox Couple Stabilize Lithium Metal Anode and Rejuvenate the Inactive Lithium in Carbonate-Based Electrolyte[J]. ADVANCED FUNCTIONAL MATERIALS,2022,32.

Wen, Zuxin.,Fang, Wenqiang.,Wu, Xiaoyu.,Qin, Zuoyu.,Kang, Hong.,...&Chen, Gen.(2022).High-Concentration Additive and Triiodide/Iodide Redox Couple Stabilize Lithium Metal Anode and Rejuvenate the Inactive Lithium in Carbonate-Based Electrolyte.ADVANCED FUNCTIONAL MATERIALS,32.

Wen, Zuxin,et al."High-Concentration Additive and Triiodide/Iodide Redox Couple Stabilize Lithium Metal Anode and Rejuvenate the Inactive Lithium in Carbonate-Based Electrolyte".ADVANCED FUNCTIONAL MATERIALS 32(2022).