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In Situ Construction of Uniform and Robust Cathode–Electrolyte Interphase for Li-Rich Layered Oxides

Journal Article · · Advanced Functional Materials
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  1. Beijing Univ. of Technology (China)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States); Stanford Univ., CA (United States); Imam AbduIrahman Bin Faisal Univ. (IAU), Dammam (Saudi Arabia)
+ Show Author Affiliations

The high-energy-density Li-rich layered oxides (LLOs) as promising cathodes for Li-ion batteries suffer from the dissolution of transition metals (especially manganese) and severe side reactions in conventional electrolytes, which greatly deteriorate their electrochemical performance. Herein, an in situ “anchoring + pouring” synergistic cathode-electrolyte interphase (CEI) construction is realized by using 1,3,6-hexanetricarbonitrile (HTCN) and tris(trimethylsilyl) phosphate (TMSP) electrolyte additives to alleviate the challenges of an LLO (Li1.13Mn0.517Ni0.256Co0.097O2). HTCN with three nitrile groups can tightly anchor transition metals by coordinative interaction to form the CEI framework, and TMSP will electrochemically decompose to reshape the CEI layer. The uniform and robust in situ constructed CEI layer can suppress the transition metal dissolution, shield the cathode against diverse side reactions, and significantly improve the overall electrochemical performance of the cathode with a discharge voltage decay of only 0.5 mV/cycle-1. Further investigations based on a series of experimental techniques and theoretical calculations have revealed the composition of in situ constructed CEI layers and their distribution, including the enhanced HTCN anchoring effect after lattice densification of LLOs. Finally, this study provides insights into the in situ CEI construction for enhancing the performance of high-energy and high-voltage cathode materials through effective, convenient and economical electrolyte approaches.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Natural Science Foundation of China (NSFC); National Key Research and Development Program of China; Beijing Municipal Education Commission; Beijing Natural Science Foundation
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1812754
Alternate ID(s):
OSTI ID: 23116408
Journal Information:
Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 8 Vol. 31; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

25 ENERGY STORAGE
Li-rich layered oxides
cathode–electrolyte interphase
in situ construction
lithium-ion batteries
voltage decay