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Title: Pulsed Laser Deposition and Characterization of Heteroepitaxial LiMn 2O 4/La 0.5Sr 0.5CoO 3 Bilayer Thin Films as Model Lithium Ion Battery Cathodes

Epitaxial LiMn 2O 4 (LMO)/La 0.5Sr 0.5CoO 3 (LSCO) bilayer thin films were grown on single crystalline SrTiO 3 (STO) (111) substrates as model lithium ion battery cathodes. The LSCO layer was used as an electrically conducting buffer layer for electrochemical testing. The LMO and LSCO layers were both epitaxial, with sub-nano flat LMO/LSCO interfaces as seen by X-ray diffraction, synchrotron X-ray scattering, and high-resolution transmission electron microscopy (HRTEM), but with a large LMO surface roughness due to the relatively large lattice mismatch with LSCO. Three-dimensional islands and depressions were formed on the strain-relaxed LMO layer, and misfit dislocations at the LMO/LSCO interface were discerned through HRTEM imaging, suggesting a Stranski–Krastanov (SK) mode thin-film growth. A crystalline structural change from cubic spinel at the LMO surface and interior to tetragonal oxygen-deficient LMO at the LMO/LSCO interface was examined. Furthermore, electrochemical tests along with in situ synchrotron X-ray scattering measurements on the epitaxial LMO/LSCO bilayers showed a significant loss of capacity after the first cycle, which was attributed to an electrical conductivity loss of the LSCO buffer layer due to irreversible lattice oxygen loss.
Authors:
ORCiD logo [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1] ; ORCiD logo [1] ;  [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
ACS Applied Nano Materials
Additional Journal Information:
Journal Volume: 1; Journal Issue: 2; Journal ID: ISSN 2574-0970
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; LiMn2O4; characterization; conductive buffer layer; crystal structure; hetero-epitaxial thin film; interface; lithium ion battery
OSTI Identifier:
1483643

Yu, Xiankai, Chen, Xiao, Buchholz, D. Bruce, Li, Qianqian, Wu, Jinsong, Fenter, Paul A., Bedzyk, Michael J., Dravid, Vinayak P., and Barnett, Scott A.. Pulsed Laser Deposition and Characterization of Heteroepitaxial LiMn2O4/La0.5Sr0.5CoO3 Bilayer Thin Films as Model Lithium Ion Battery Cathodes. United States: N. p., Web. doi:10.1021/acsanm.7b00133.
Yu, Xiankai, Chen, Xiao, Buchholz, D. Bruce, Li, Qianqian, Wu, Jinsong, Fenter, Paul A., Bedzyk, Michael J., Dravid, Vinayak P., & Barnett, Scott A.. Pulsed Laser Deposition and Characterization of Heteroepitaxial LiMn2O4/La0.5Sr0.5CoO3 Bilayer Thin Films as Model Lithium Ion Battery Cathodes. United States. doi:10.1021/acsanm.7b00133.
Yu, Xiankai, Chen, Xiao, Buchholz, D. Bruce, Li, Qianqian, Wu, Jinsong, Fenter, Paul A., Bedzyk, Michael J., Dravid, Vinayak P., and Barnett, Scott A.. 2018. "Pulsed Laser Deposition and Characterization of Heteroepitaxial LiMn2O4/La0.5Sr0.5CoO3 Bilayer Thin Films as Model Lithium Ion Battery Cathodes". United States. doi:10.1021/acsanm.7b00133. https://www.osti.gov/servlets/purl/1483643.
@article{osti_1483643,
title = {Pulsed Laser Deposition and Characterization of Heteroepitaxial LiMn2O4/La0.5Sr0.5CoO3 Bilayer Thin Films as Model Lithium Ion Battery Cathodes},
author = {Yu, Xiankai and Chen, Xiao and Buchholz, D. Bruce and Li, Qianqian and Wu, Jinsong and Fenter, Paul A. and Bedzyk, Michael J. and Dravid, Vinayak P. and Barnett, Scott A.},
abstractNote = {Epitaxial LiMn2O4 (LMO)/La0.5Sr0.5CoO3 (LSCO) bilayer thin films were grown on single crystalline SrTiO3 (STO) (111) substrates as model lithium ion battery cathodes. The LSCO layer was used as an electrically conducting buffer layer for electrochemical testing. The LMO and LSCO layers were both epitaxial, with sub-nano flat LMO/LSCO interfaces as seen by X-ray diffraction, synchrotron X-ray scattering, and high-resolution transmission electron microscopy (HRTEM), but with a large LMO surface roughness due to the relatively large lattice mismatch with LSCO. Three-dimensional islands and depressions were formed on the strain-relaxed LMO layer, and misfit dislocations at the LMO/LSCO interface were discerned through HRTEM imaging, suggesting a Stranski–Krastanov (SK) mode thin-film growth. A crystalline structural change from cubic spinel at the LMO surface and interior to tetragonal oxygen-deficient LMO at the LMO/LSCO interface was examined. Furthermore, electrochemical tests along with in situ synchrotron X-ray scattering measurements on the epitaxial LMO/LSCO bilayers showed a significant loss of capacity after the first cycle, which was attributed to an electrical conductivity loss of the LSCO buffer layer due to irreversible lattice oxygen loss.},
doi = {10.1021/acsanm.7b00133},
journal = {ACS Applied Nano Materials},
number = 2,
volume = 1,
place = {United States},
year = {2018},
month = {1}
}