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Engineering lithium-ion battery cathodes for high-voltage applications using electromagnetic excitation

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Abstract

Microwave radiation (MWR), a type of electromagnetic excitation source, reduces the synthesis temperature and processing time for chemical reactions compared to traditional synthesis methods. Recently, we demonstrated that MWR can engineer ceramics with different crystal phases compared to traditional methods [Journal of Materials Chemistry A5, 35 (2017)]. In this study, we further apply the MWR-assisted technique to improve the electrochemical performance of LiCoO2 cathodes by engineering TiO2 and ZrO2 ceramic coatings. Electrochemical tests suggest that the TiO2 coating improves the rate capability of the LiCoO2 electrode. Both TiO2 and ZrO2 coatings improve the high-voltage (4.5 V) cycling stability of LiCoO2. The capacity remaining is improved from 52.8 to 84.4% and 81.9% by the TiO2 coating and the ZrO2 coating, respectively, after 40 cycles. We compare these results with existing studies that apply traditional methods to engineer TiO2/ZrO2 on LiCoO2, and find that the MWR-assisted method shows better performance improvement. X-ray photoelectron spectroscopy measurements suggest that the improved cycling stability arises from the formation of metal fluorides that protect the electrode from side reactions with electrolytes. This mechanism is further supported by the reduced Co dissolution from TiO2/ZrO2-coated LiCoO2 electrode after cycling. This study provides a new toolbox facilitating the integration of many delicate, low melting point materials like polymers into battery electrodes.

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Acknowledgements

This work was supported by National Science Foundation (NSF) CAREER Award (CMMI1751605) and INCUBATE seed funding from Carnegie Mellon University. Microwave field-assisted TiO2 synthesis efforts were supported by the DARPA AIRA Program (Grant Number HR00111990030). The authors acknowledge use of the Materials Characterization Facility at Carnegie Mellon University supported by Grant MCF-677,785. The Authors thank Dr. Joel Gillespie from the University of Pittsburgh Materials Characterization Laboratory for the access to the XPS spectrometer. Dr. Haiyan Wang and Ms. Xin Li Phuah acknowledge the support from the Office of Naval Research under Contract Nos. 1. N00014-17-1-2087 and N00014-16-1-2778. This research used 6-ID-D beamline and other resources in Advanced Photon Source, Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

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Authors and Affiliations

  1. Department of Mechanical Engineering, Carnegie Mellon University, Pittsburgh, PA, USA

    Laisuo Su, Shikhar Krishn Jha, Nathan Nakamura & B. Reeja-Jayan

  2. School of Materials Engineering, Purdue University, West Lafayette, IN, USA

    Xin Li Phuah & Haiyan Wang

  3. Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, PA, USA

    Jiang Xu

  4. Advanced Photo Source, Argonne National Laboratory, Lemont, IL, USA

    John S. Okasinski

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  1. Laisuo Su
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  2. Shikhar Krishn Jha
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  3. Xin Li Phuah
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  4. Jiang Xu
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  5. Nathan Nakamura
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  6. Haiyan Wang
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  7. John S. Okasinski
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  8. B. Reeja-Jayan
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Contributions

LS contributed to conceptualization, experimental design, carrying out measurements, manuscript composition. SKJ helped in carrying out measurements. XLP involved in carrying out measurements. JX contributed to carrying out measurements. NN helped in experimental design, manuscript composition. HW helped in resources, funding acquisition. JSO contributed to resources. BRJ helped in supervision, experimental design, resources, manuscript composition, funding acquisition.

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Correspondence to B. Reeja-Jayan.

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Su, L., Jha, S.K., Phuah, X.L. et al. Engineering lithium-ion battery cathodes for high-voltage applications using electromagnetic excitation. J Mater Sci 55, 12177–12190 (2020). https://doi.org/10.1007/s10853-020-04871-5

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