4.8 Article

Stable Electrode/Electrolyte Interface for High-Voltage NCM 523 Cathode Constructed by Synergistic Positive and Passive Approaches

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 48, Pages 57107-57117

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c15690

Keywords

lithium-ion battery; high-voltage electrolyte; NCM 523 cathode; lithium sulfide; cathode electrolyte interface; additive

Funding

  1. National Natural Science Foundation of China [21773279, 22075305, 52061135110]
  2. Zhejiang Province Public Welfare Technology Application Research Project [LGG19B010001]
  3. Key Research Program of the Chinese Academy of Sciences [ZDRW_CN_2020-1]
  4. Ningbo Science & Technology Innovation 2025 Major Project [2019B10050, 2019B10113, 2020Z024, 2020Z101, 2020Z025]
  5. Key Laboratory of Biobased Polymeric Materials of Zhejiang Province

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A new synergistic positive and passive approach is proposed to construct a stable electrode-electrolyte interface at high voltage in lithium-ion batteries, resulting in significantly improved cyclic stability and capacity retention by adding small amounts of Li2S and AN. This study provides new principles guiding high-voltage lithium-ion batteries with excellent electrochemical performance.
Increasing the working voltage of lithium-ion batteries (LIBs) is an efficient way to increase energy density. However, high voltage triggers excessive electrolyte decomposition at the electrode-electrolyte interfaces, where the electrochemical performance such as cyclic stability and rate capability is seriously deteriorated. A new synergistic positive and passive approach is proposed in this work to construct a stable electrode-electrolyte interface at high voltage. As a positive approach, inorganic lithium sulfide salt (Li2S) is used as an electrolyte additive to build a stable cathode electrolyte interface (CEI) at the LiNi0.5Co0.2Mn0.3O2 (NCMS23) cathode surface. In a passive way, acetonitrile (AN) is applied as a solvent additive to suppress oxidative decomposition of a carbonate electrolyte via preferential solvation with a lithium ion. Because of the synergistic interaction between the positive and passive approaches, the cyclic stabilities of NCMS23/Li cells improved with a tiny amount of Li2S (0.01 mg mL(-1)) and AN (0.5 vol %). The capacity retention increased to 80.74% after 200 cycles compared to the cells with the blank electrolyte (67.98%) and AN-containing electrolyte (75.8%). What is more, the capacity retention of the NCM523/graphite full cell is increased from 65 to 81% with the addition of the same amount of Li2S and AN after 180 cycles. The mechanism is revealed on the basis of the theoretical calculations and various characterizations. The products derived from the preferential adsorption and oxidation of Li2S on the surface of NCM523 effectively increase the content of inorganic ingredients. However, the presence of AN prevents oxidation of the solvent. This study provides new principle guiding studies on a high-voltage lithium-ion battery with excellent electrochemical performance.

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