4.6 Article

Sulfonate-Based Artificial Cathode-Electrolyte Interface to Enhance Electrochemical Performance of Ni-Rich Layered Oxide Cathode Materials

Journal

ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 8, Issue 19, Pages 7316-7323

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.0c00404

Keywords

lithium-ion batteries; nickel-rich cathode; cathode-electrolyte interface; ammonium sulfate; surface

Funding

  1. Basic Science Research Program through the National Research Foundation of Korea (NRF) - Ministry of Education [NRF-2017R1A6A1A06015181]
  2. National Research Foundation of Korea (NRF) - Korea government (MSIP) [2017M1A2A2044506, 2019R1C1C1002249]
  3. National Research Foundation of Korea [2019R1C1C1002249] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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Despite significant progress in the field of Li-ion battery development over the past 30 years, challenges associated with the gradual shift from small-scale to large-scale battery applications necessitate the search for better electrode materials. In particular, Ni-rich layered oxide cathode materials (NCM) feature high specific capacities but suffer from inferior high-temperature cycling performance because of poor surface stability. Herein, we use ammonium sulfate (AS) to form a bifunctionalized cathode-electrolyte interface and thus improve NCM surface stability, revealing that thermal treatment of NCM in the presence of AS affords an artificial cathode-electrolyte interface comprising sulfonate and amino functional groups and thus effectively hinders electrolyte decomposition and Ni dissolution. The modified NCM feature surfaces with well-developed artificial cathode- electrolyte interfaces (which do not compromise structural stability) exhibit good high-temperature cycling performance. The modified NCM at 400 degrees C features a capacity retention of 75.6% after 100 cycles at 45 degrees C, whereas a much lower value of 52.2% is observed for the bare counterpart under identical conditions. Cycling- induced electrolyte decomposition, cracking, and Ni dissolution are strongly suppressed in cells with surface-modified NCM, which implies that residual hydrogen fluoride removal by the bifunctionalized artificial cathode-electrolyte interface improves NCM surface stability. Thus, the use of a bifunctionalized artificial cathode-electrolyte interface modified by task-specific AS is concluded to improve the surface properties of NCM and their high-temperature electrochemical performance.

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