Journal
APPLIED ENERGY
Volume 299, Issue -, Pages -Publisher
ELSEVIER SCI LTD
DOI: 10.1016/j.apenergy.2021.117315
Keywords
Lithium-ion battery; X-ray scattering; Transmission X-ray microscopy; Operando measurement; Electro-chemo-mechanical behavior; Surface engineering
Categories
Funding
- National Science Foundation (NSF) CAREER Award [CMMI1751605]
- Scott Institute Seed Grants
- Carnegie Mellon University
- National Defense Science and Engineering Graduate (NDSEG) Fellowship
- National Science Foundation [DEAC0206CH11357]
- Advanced Photon Source, Argonne National Laboratory [DEAC0206CH11357]
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This study utilizes multiscale operando techniques to investigate battery electrodes, integrating synchrotron X-ray scattering and high-resolution transmission X-ray microscopy. Through an over-lithiation test of LiCoO2 electrodes, the complementarity of the two operando techniques is demonstrated, and the mechanism of the polymer coating in improving cycling stability is discovered.
The electrochemical performance and cycle life of lithium-ion batteries (LIBs) depend on the electrochemical, chemical, and mechanical behavior of electrodes and electrolytes. Despite extensive studies conducted previously, challenges exist to decouple these behaviors, capture the evolution of electro-chemo-mechanical behavior in realistic conditions, and correlate atomic-scale stress evolution to micro-scale bulk mechanical degradation. Here, we report multiscale operando techniques to investigate polydisperse battery electrodes by integrating volume-averaged quantitative synchrotron X-ray scattering with high-resolution transmission X-ray microscopy (TXM). The former provides us information spanning a wide spatial range, from Angstrom-level atomic structures to micrometer-level particle scales, while the latter provides time-resolved 2D images of the particles during cycling. The complementarity of the two operando techniques is demonstrated by an over-lithiation test of LiCoO2 electrodes, where particles crack and eventually pulverize. Additionally, the techniques are applied to study LiCoO2 cycling stability from 3.0 V to 4.5 V. Operando X-ray scattering result shows nanometer-scale Applied Energy 299 (2021) features keep forming in LiCoO2 electrodes during cycling, resulting in an increased projected area observed by the TXM experiment. The formation of such features is inhibited by a polymer coating on the electrode, leading to vastly improved cycling stability. The polymer coating alleviates LiCoO2 surface deterioration, reduces side product generation, and inhibits LiCoO2 particles volume expansion during the cycling test. These operando multimodal X-ray techniques presented herein thus offer a novel, multiscale diagnostic modality for studying existing and emerging battery materials, aiding the development of next-generation LIBs.
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