Abstract
High-capacity cathodes (LiNi0.8Mn0.1Co0.1O2, NMC811) are promising for vehicle electrification because of their high gravimetric energy density. However, their electrochemical performance still relies upon the stability of the cathode electrolyte interphase (CEI). A highly reactive cathode interface leads to parasitic side reactions with electrolytes, resulting in accelerated capacity fading. Well-developed LiF and LiF-like inorganic compounds are believed to be good CEI components for stabilizing such reactive electrode interfaces. However, it is challenging to form an optimal surface sub-nanolayer of LiF on the cathode surfaces because of the complexity of the electrochemical reaction during battery cycling. Herein, the formation of a conformal LiF layer on the NMC811 electrode surface via an in situ ion-exchange metathesis process is reported, demonstrating a promising electrochemical performance because of a LiF-stabilized CEI. In situ generated LiF-coated NMC811 electrodes exhibit ≈97% capacity retention up to 100 cycles at a 0.3 C rate with average coulombic efficiency of ≈99.9% and ≈80% capacity retention up to 200 cycles at a 1 C rate with average coulombic efficiency of >99.6%. This finding may pave the way for reengineering the CEI to enhance the electrochemical performances and cycling stability of the high-capacity cathodes.
| Original language | English |
|---|---|
| Article number | 2302443 |
| Journal | Advanced Functional Materials |
| Volume | 33 |
| Issue number | 44 |
| DOIs | |
| State | Published - Oct 25 2023 |
Funding
This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract number DE-AC05-00OR22725 with the US Department of Energy (DOE). The STEM-EDS analysis of this work was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. This manuscript has been authored by UT-Battelle, LLC, under contract number DE-AC05_00OR22725, with US Department of Energy (DOE). The United States Goverment retains and the publisher, by accepting the article for publication, acknowledges that the United States Goverment retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Goverment purposes. The DOE will provide public access to these results of federally sponsored research under the DOE Public Access Plan (http://energy>gov/downloads/doepublic-access-plan). This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract number DE‐AC05‐00OR22725 with the US Department of Energy (DOE). The STEM‐EDS analysis of this work was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. This manuscript has been authored by UT‐Battelle, LLC, under contract number DE‐AC05_00OR22725, with US Department of Energy (DOE). The United States Goverment retains and the publisher, by accepting the article for publication, acknowledges that the United States Goverment retains a non‐exclusive, paid‐up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Goverment purposes. The DOE will provide public access to these results of federally sponsored research under the DOE Public Access Plan (http://energy>gov/downloads/doepublic‐access‐plan).
Keywords
- NMC811
- conformal LiF
- high energy density batteries
- high-capacity cathodes
- in situ ion-exchange metathesis
