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Title: Electrochemical properties and structural evolution of O3-type layered sodium mixed transition metal oxides with trivalent nickel

Abstract

The electrochemical properties of NaNi0.5Co0.5O2 and NaNi0.5Fe0.5O2 and their structural transitions as a function of Na extraction associated with redox reactions are investigated. Synthesized in the O3-type layered structure, both materials show reasonable electrochemical activities at room temperature, delivering approximately 0.5 Na per formula unit at C/10 discharge. More Na can be reversibly cycled in NaNi0.5Co0.5O2 at elevated temperature and/or in an extended voltage window, while NaNi0.5Fe0.5O2 shows significant capacity fading at a high voltage cutoff which is likely due to Fe4+ migration. In situ X-ray diffraction shows that the structural changes in the two materials upon desodiation are very different. NaNi0.5Co0.5O2 goes through many different two-phase reactions including three different O3-type and three different P3-type structures during cycling, producing a voltage profile with multiple plateau-like features. In contrast, NaNi0.5Fe0.5O2 has a smooth voltage profile and shows the typical O3–P3 phase transition without lattice distortion seen in other materials. Finally, this different structural evolution upon desodiation and re-sodiation can be explained by the electronic structure of the mixed transition metals and how it perturbs the ordering between Na ions differently.

Authors:
 [1];  [2];  [1];  [2];  [2];  [3]; ORCiD logo [4]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
  2. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering; Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF); Samsung Advanced Inst. of Technology (Korea, Republic of)
OSTI Identifier:
1475004
Grant/Contract Number:  
AC02-05CH11231; ACI-1053575
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 5; Journal Issue: 9; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Vassilaras, Plousia, Kwon, Deok-Hwang, Dacek, Stephen T., Shi, Tan, Seo, Dong-Hwa, Ceder, Gerbrand, and Kim, Jae Chul. Electrochemical properties and structural evolution of O3-type layered sodium mixed transition metal oxides with trivalent nickel. United States: N. p., 2017. Web. doi:10.1039/c6ta09220a.
Vassilaras, Plousia, Kwon, Deok-Hwang, Dacek, Stephen T., Shi, Tan, Seo, Dong-Hwa, Ceder, Gerbrand, & Kim, Jae Chul. Electrochemical properties and structural evolution of O3-type layered sodium mixed transition metal oxides with trivalent nickel. United States. doi:10.1039/c6ta09220a.
Vassilaras, Plousia, Kwon, Deok-Hwang, Dacek, Stephen T., Shi, Tan, Seo, Dong-Hwa, Ceder, Gerbrand, and Kim, Jae Chul. Mon . "Electrochemical properties and structural evolution of O3-type layered sodium mixed transition metal oxides with trivalent nickel". United States. doi:10.1039/c6ta09220a. https://www.osti.gov/servlets/purl/1475004.
@article{osti_1475004,
title = {Electrochemical properties and structural evolution of O3-type layered sodium mixed transition metal oxides with trivalent nickel},
author = {Vassilaras, Plousia and Kwon, Deok-Hwang and Dacek, Stephen T. and Shi, Tan and Seo, Dong-Hwa and Ceder, Gerbrand and Kim, Jae Chul},
abstractNote = {The electrochemical properties of NaNi0.5Co0.5O2 and NaNi0.5Fe0.5O2 and their structural transitions as a function of Na extraction associated with redox reactions are investigated. Synthesized in the O3-type layered structure, both materials show reasonable electrochemical activities at room temperature, delivering approximately 0.5 Na per formula unit at C/10 discharge. More Na can be reversibly cycled in NaNi0.5Co0.5O2 at elevated temperature and/or in an extended voltage window, while NaNi0.5Fe0.5O2 shows significant capacity fading at a high voltage cutoff which is likely due to Fe4+ migration. In situ X-ray diffraction shows that the structural changes in the two materials upon desodiation are very different. NaNi0.5Co0.5O2 goes through many different two-phase reactions including three different O3-type and three different P3-type structures during cycling, producing a voltage profile with multiple plateau-like features. In contrast, NaNi0.5Fe0.5O2 has a smooth voltage profile and shows the typical O3–P3 phase transition without lattice distortion seen in other materials. Finally, this different structural evolution upon desodiation and re-sodiation can be explained by the electronic structure of the mixed transition metals and how it perturbs the ordering between Na ions differently.},
doi = {10.1039/c6ta09220a},
journal = {Journal of Materials Chemistry. A},
number = 9,
volume = 5,
place = {United States},
year = {2017},
month = {1}
}

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