Identifying the chemical and structural irreversibility in LiNi0.8Co0.15Al0.05O2-a model compound for classical layered intercalation

Haodong Liu, Hao Liu, Ieuan D. Seymour, Natasha Chernova, Kamila M. Wiaderek, Nicole M. Trease, Sunny Hy, Yan Chen, Ke An, Minghao Zhang, Olaf J. Borkiewicz, Saul H. Lapidus, Bao Qiu, Yonggao Xia, Zhaoping Liu, Peter J. Chupas, Karena W. Chapman, M. Stanley Whittingham, Clare P. Grey, Ying Shirley Meng* (Corresponding Author)

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

49 Citations (Scopus)


In this work, we extracted 95% of the electrochemically available Li from LiNi0.8Co0.15Al0.05O2 (NCA) by galvanostatically charging the NCA/MCMB full cell to 4.7 V. Joint powder X-ray and neutron diffraction (XRD & ND) studies were undertaken for NCA at highly charged states at the first cycle, and discharged states at different cycles. The results indicate that the bulk structure of NCA maintains the O3 structure up to the extraction of 0.90 Li per formula unit. In addition, we found that the transition metal layer becomes more disordered along the c-axis than along the a- and b-axes upon charging. This anisotropic disorder starts to develop no later than 4.3 V on charge and continues to grow until the end of charge. As Li is re-inserted during discharge, the structure that resembles the pristine NCA is recovered. The irreversible loss of Li and the migration of Ni to the Li layer have been quantified by the joint XRD and ND refinement and the results were further verified by solid state 7Li NMR and magnetic measurements. Our work clearly demonstrates that the NCA bulk retains a robust, single phase O3 structure throughout the wide delithiation range (up to 0.9 Li per formula unit of NCA) and is suitable for higher energy density usage with proper modifications.

Original languageEnglish
Pages (from-to)4189-4198
Number of pages10
JournalJournal of Materials Chemistry A
Issue number9
Publication statusPublished - 7 Feb 2018

Bibliographical note

Funding Information:
This work was supported by the NorthEast Center for Chemical Energy Storage (NECCES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award no. DE-SC0012583. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357 and the resources of the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The neutron experiments benefited from the SNS user facility, sponsored by the office of Basic Energy Sciences (BES), the Office of Science of the DOE.

Funding Information:
This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (

Publisher Copyright:
© 2018 The Royal Society of Chemistry.


Dive into the research topics of 'Identifying the chemical and structural irreversibility in LiNi0.8Co0.15Al0.05O2-a model compound for classical layered intercalation'. Together they form a unique fingerprint.

Cite this