Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 14, Pages 16245-16257Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c01245
Keywords
lithium-ion battery; PDMS binder; NCM 523 cathode; cross-linking; cathode-electrolyte interface
Funding
- National Natural Science Foundation of China [52061135110, 5187052685, 21773279, 22075305]
- Natural Science Foundation of Zhejiang Province [LD22E020003]
- Shanxi Provincial Natural Science Foundation of China [201801D121085]
- Key Research Program of the Chinese Academy of Sciences [ZDRW_CN_2020-1]
- Ningbo Science & Technology Innovation 2025 Major Project [2019B10050, 2019B10113, 2020Z024, 2020Z101, 2020Z025]
- Key Laboratory of Bio-based Polymeric Materials of Zhejiang Province
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By incorporating PDMS binder into the electrode, the electrode-electrolyte interface of lithium-ion batteries can be stabilized at high voltage, leading to improved cycling performance and rate performance.
Increasing working voltage is a promising way to increase the energy density of lithium-ion batteries. Cycling and rate performance deteriorated due to excessive electrolyte decomposition and uncontrolled formation of a cathode-electrolyte interface (CEI) layer at a high voltage. A new concept is proposed to construct a high-voltage-stable electrode-electrolyte interface. An elastomeric poly(dimethyl siloxane) (PDMS) binder is incorporated into the electrode to modify the LiNi0.5Co0.2Mn0.3O2 (NCM 523) particle surface via an in situ cross-linking reaction between hydroxy-terminated PDMS and methyl trimethoxy silane promoted by moisture at ambient conditions (MPDMS). Improved electrochemical performance is achieved with the MPDMS binder in terms of reversible capacity (201 vs 185 mAh.g(-1) at 0.2C), capacity retention (80 vs 68%, after 300 cycles at 1C), and rate performance (55.6% increase at 5C), as demonstrated by the NCM 523 parallel to Li half-cell. The NCM 523 parallel to graphite full-cell also shows improved performance at 4.6 V (147 vs 128 mAh.g(-1), 82 vs 76%, after 200 cycles at 1C). The mechanism studies indicate that MPDMS exerts multiple effects, including cathode surface passivation, solvation structure tuning, electrolyte uptake enhancement, and mechanical stress relief. This work provides an inspiring route to realize high-voltage application of lithium-ion battery technology.
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