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author:

Hu, G. (Hu, G..) [1] | Yang, Z. (Yang, Z..) [2] | Zhang, X. (Zhang, X..) [3] | Liu, Y. (Liu, Y..) [4] | Lin, Y. (Lin, Y..) [5] | Chen, S. (Chen, S..) [6] | Chen, Y. (Chen, Y..) [7] | Sa, B. (Sa, B..) [8] | Zhang, Y. (Zhang, Y..) [9]

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Scopus

Abstract:

The electrolyte in lithium-metal batteries (LMBs) plays a pivotal role in stabilizing the surface of the lithium metal anode (LMA) and high-voltage cathode. However, currently widely studied ether-based electrolytes, although it has good compatibility with LMA due to their lower reactivity, are facing significant challenges related to poor oxidation resistance and cathode/electrolyte interface (CEI) instability when combined with the high-voltage cathode, particularly at elevated temperatures. Therefore, there is an urgent need to design advanced electrolytes capable of maintaining high stability under high-voltage and high-temperature conditions. Here, we have developed an ultra-stable localized high-concentration electrolyte (LHCE) by introducing triethylene glycol dimethyl ether (TG), which exhibits strong solvation ability. Computational and experimental results demonstrate that the designed TG-based dilute high-concentration electrolyte (TG-DHCE) possesses a stable solvation structure, high oxidation resistance, and thermal stability, making it ideal for LMBs. Furthermore, the unique solvation structure of TG-DHCE promotes the preferential decomposition of anions while facilitating the formation of stable, inorganic-rich electrode/electrolyte interfaces on the anode and cathode. Consequently, equipped with TG-DHCE, Li||Li cells (more than 1600 h) and Li||NCM523 cells (80.6%, 250 cycles) show superior stability and also demonstrate remarkable performance even at elevated temperatures (60 °C). Additionally, under the harsh conditions of ultrahigh loading NCM523 cathode (19.7 mg/cm2) and limited Li reservoir (twice excess Li was deposited on Cu, Li@Cu) (N/P = 2), Li@Cu||NCM523 cells still maintain stable operation. This work pioneers a new path by choosing strongly solvating solvents, effectively enhancing the cycle life of LMBs under high-voltage and high-temperature conditions. © 2024

Keyword:

High-temperature High-voltage Localized high-concentration electrolyte Stable solvation structure Strong solvation ability

Community:

  • [ 1 ] [Hu G.]College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 2 ] [Hu G.]Fujian College, University of Chinese Academy of Sciences, 155 Yangqiao Road West, Fujian, Fuzhou, 350002, China
  • [ 3 ] [Yang Z.]Key Laboratory of Eco-materials Advanced Technology, College of Materials Science and Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
  • [ 4 ] [Zhang X.]Fujian College, University of Chinese Academy of Sciences, 155 Yangqiao Road West, Fujian, Fuzhou, 350002, China
  • [ 5 ] [Liu Y.]Fujian College, University of Chinese Academy of Sciences, 155 Yangqiao Road West, Fujian, Fuzhou, 350002, China
  • [ 6 ] [Lin Y.]School of Science and Engineering, The Chinese University of Hong Kong, Guangdong, Shenzhen, 518172, China
  • [ 7 ] [Chen S.]Fujian College, University of Chinese Academy of Sciences, 155 Yangqiao Road West, Fujian, Fuzhou, 350002, China
  • [ 8 ] [Chen S.]University of Chinese Academy of Sciences, Beijing, 100049, China
  • [ 9 ] [Chen Y.]Fujian College, University of Chinese Academy of Sciences, 155 Yangqiao Road West, Fujian, Fuzhou, 350002, China
  • [ 10 ] [Chen Y.]University of Chinese Academy of Sciences, Beijing, 100049, China
  • [ 11 ] [Sa B.]Key Laboratory of Eco-materials Advanced Technology, College of Materials Science and Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
  • [ 12 ] [Zhang Y.]Fujian College, University of Chinese Academy of Sciences, 155 Yangqiao Road West, Fujian, Fuzhou, 350002, China
  • [ 13 ] [Zhang Y.]Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fujian, Fuzhou, 350108, China
  • [ 14 ] [Zhang Y.]University of Chinese Academy of Sciences, Beijing, 100049, China

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Source :

Energy Storage Materials

ISSN: 2405-8297

Year: 2024

Volume: 69

1 8 . 9 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 1

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 3

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