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Title: Surface Characterization of Li-Substituted Compositionally Heterogeneous NaLi 0.045Cu 0.185Fe 0.265Mn 0.505O 2 Sodium-Ion Cathode Material

Abstract

The understanding of surface chemical and structural processes can provide some insights into designing stable sodium cathode materials. Herein, Li-substituted and compositionally heterogeneous NaLi 0.045Cu 0.185Fe 0.265Mn 0.505O 2 is used as a platform to investigate the interplay between Li substitution, surface chemistry, and battery performance. Li substitution improves the initial discharge capacity and energy density. Yet, there is no noticeable benefit in the long-term cycling stability of this material. The Li substitution in the transition-metal (TM) layer also seems to influence the transition-metal (TM) 3d–oxygen (O) 2p hybridization. Upon desodiation, the surface of active particles undergoes significant transition-metal reduction, especially Mn. Furthermore, the presence of electrolyte drastically accelerates such surface degradation. In general, the Li-substituted material experiences severe surface degradation, which is partially responsible for the performance degradation upon long-term cycling. While some studies have introduced the benefits of Li substitution, the present study suggests that the effectiveness of the Li substitution strategy depends on the TM compositional distribution. More efforts are needed to improve the surface chemistry of Li-substituted sodium cathode materials.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [5];  [1];  [3];  [3]; ORCiD logo [6];  [3];  [3]; ORCiD logo [1]
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  2. Tianjin Univ., (China); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Chinese Academy of Sciences (CAS), Dongguan (China). Dongguan Inst. of Neutron Science; Australian Nuclear Science and Technology Organisation (ANSTO), Lucas Heights, NSW (Australia)
  5. Australian Nuclear Science and Technology Organisation (ANSTO), Lucas Heights, NSW (Australia)
  6. Tianjin Univ., (China)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1528857
Grant/Contract Number:  
AC02-76SF00515; 11805034; 21704105
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 123; Journal Issue: 18; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English

Citation Formats

Rahman, Muhammad Mominur, Zhang, Yan, Xia, Sihao, Kan, Wang Hay, Avdeev, Maxim, Mu, Linqin, Sokaras, Dimosthenis, Kroll, Thomas, Du, Xi-Wen, Nordlund, Dennis, Liu, Yijin, and Lin, Feng. Surface Characterization of Li-Substituted Compositionally Heterogeneous NaLi0.045Cu0.185Fe0.265Mn0.505O2 Sodium-Ion Cathode Material. United States: N. p., 2019. Web. doi:10.1021/acs.jpcc.9b01126.
Rahman, Muhammad Mominur, Zhang, Yan, Xia, Sihao, Kan, Wang Hay, Avdeev, Maxim, Mu, Linqin, Sokaras, Dimosthenis, Kroll, Thomas, Du, Xi-Wen, Nordlund, Dennis, Liu, Yijin, & Lin, Feng. Surface Characterization of Li-Substituted Compositionally Heterogeneous NaLi0.045Cu0.185Fe0.265Mn0.505O2 Sodium-Ion Cathode Material. United States. doi:10.1021/acs.jpcc.9b01126.
Rahman, Muhammad Mominur, Zhang, Yan, Xia, Sihao, Kan, Wang Hay, Avdeev, Maxim, Mu, Linqin, Sokaras, Dimosthenis, Kroll, Thomas, Du, Xi-Wen, Nordlund, Dennis, Liu, Yijin, and Lin, Feng. Thu . "Surface Characterization of Li-Substituted Compositionally Heterogeneous NaLi0.045Cu0.185Fe0.265Mn0.505O2 Sodium-Ion Cathode Material". United States. doi:10.1021/acs.jpcc.9b01126.
@article{osti_1528857,
title = {Surface Characterization of Li-Substituted Compositionally Heterogeneous NaLi0.045Cu0.185Fe0.265Mn0.505O2 Sodium-Ion Cathode Material},
author = {Rahman, Muhammad Mominur and Zhang, Yan and Xia, Sihao and Kan, Wang Hay and Avdeev, Maxim and Mu, Linqin and Sokaras, Dimosthenis and Kroll, Thomas and Du, Xi-Wen and Nordlund, Dennis and Liu, Yijin and Lin, Feng},
abstractNote = {The understanding of surface chemical and structural processes can provide some insights into designing stable sodium cathode materials. Herein, Li-substituted and compositionally heterogeneous NaLi0.045Cu0.185Fe0.265Mn0.505O2 is used as a platform to investigate the interplay between Li substitution, surface chemistry, and battery performance. Li substitution improves the initial discharge capacity and energy density. Yet, there is no noticeable benefit in the long-term cycling stability of this material. The Li substitution in the transition-metal (TM) layer also seems to influence the transition-metal (TM) 3d–oxygen (O) 2p hybridization. Upon desodiation, the surface of active particles undergoes significant transition-metal reduction, especially Mn. Furthermore, the presence of electrolyte drastically accelerates such surface degradation. In general, the Li-substituted material experiences severe surface degradation, which is partially responsible for the performance degradation upon long-term cycling. While some studies have introduced the benefits of Li substitution, the present study suggests that the effectiveness of the Li substitution strategy depends on the TM compositional distribution. More efforts are needed to improve the surface chemistry of Li-substituted sodium cathode materials.},
doi = {10.1021/acs.jpcc.9b01126},
journal = {Journal of Physical Chemistry. C},
number = 18,
volume = 123,
place = {United States},
year = {2019},
month = {4}
}

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This content will become publicly available on April 11, 2020
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