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Title: Deciphering the Cathode-Electrolyte Interfacial Chemistry in Sodium Layered Cathode Materials

Abstract

The ever–increasing demand for stationary energy storage has driven the prosperous investigation of low–cost sodium ion batteries. The inferior long–term cycling stability of cathode materials is a significant roadblock toward the wide commercialization of sodium ion batteries. This study enlightens a path toward empowering stable sodium ion batteries through incisive diagnostics of the multiscale surface chemical processes in layered oxide materials (e.g., O3–NaNi 1/3Fe 1/3Mn 1/3O 2). The major challenges are unraveled in a promising sodium layered cathode material using a range of complementary advanced spectroscopic and imaging diagnostic techniques. It is discovered that the cathode–electrolyte interfacial reaction triggers transition metal reduction, heterogeneous surface reconstruction, metal dissolution, and formation of intragranular nanocracks. These surface chemistry driven processes are partly responsible for significant performance decay. This diagnostic study also rationalizes the elemental substitution and surface passivation methods that are widely applied in the field. The prepassivated and Ti–substituted cathode materials allow for significantly improved cycling stability by inhibiting the metal dissolution. Furthermore, incisively diagnosing the interfacial chemistry not only creates scientific insights into understanding sodium cathode chemistry, but also represents an advance toward establishing universal interfacial design principles for all alkali metal ion cathode materials.

Authors:
 [1];  [1];  [2];  [3];  [4];  [1];  [2];  [5];  [6];  [7]; ORCiD logo [1]
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Tianjin Univ., Tianjin (China); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. China Institute of Atomic Energy, Beijing (China)
  5. Tianjin Univ., Tianjin (China)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  7. Brookhaven National Lab. (BNL), Upton, NY (United States); Univ. of California, Irvine, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); Canadian Light Source, Inc.
OSTI Identifier:
1490880
Alternate Identifier(s):
OSTI ID: 1479832; OSTI ID: 1493885
Grant/Contract Number:  
AC02-76SF00515; SC0012704; AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 34; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; dissolution; heterogeneous reconstruction; interfacial chemistry; nanocrack; sodium batteries

Citation Formats

Mu, Linqin, Feng, Xu, Kou, Ronghui, Zhang, Yan, Guo, Hao, Tian, Chixia, Sun, Cheng -Jun, Du, Xi -Wen, Nordlund, Dennis, Xin, Huolin L., and Lin, Feng. Deciphering the Cathode-Electrolyte Interfacial Chemistry in Sodium Layered Cathode Materials. United States: N. p., 2018. Web. doi:10.1002/aenm.201801975.
Mu, Linqin, Feng, Xu, Kou, Ronghui, Zhang, Yan, Guo, Hao, Tian, Chixia, Sun, Cheng -Jun, Du, Xi -Wen, Nordlund, Dennis, Xin, Huolin L., & Lin, Feng. Deciphering the Cathode-Electrolyte Interfacial Chemistry in Sodium Layered Cathode Materials. United States. doi:10.1002/aenm.201801975.
Mu, Linqin, Feng, Xu, Kou, Ronghui, Zhang, Yan, Guo, Hao, Tian, Chixia, Sun, Cheng -Jun, Du, Xi -Wen, Nordlund, Dennis, Xin, Huolin L., and Lin, Feng. Tue . "Deciphering the Cathode-Electrolyte Interfacial Chemistry in Sodium Layered Cathode Materials". United States. doi:10.1002/aenm.201801975.
@article{osti_1490880,
title = {Deciphering the Cathode-Electrolyte Interfacial Chemistry in Sodium Layered Cathode Materials},
author = {Mu, Linqin and Feng, Xu and Kou, Ronghui and Zhang, Yan and Guo, Hao and Tian, Chixia and Sun, Cheng -Jun and Du, Xi -Wen and Nordlund, Dennis and Xin, Huolin L. and Lin, Feng},
abstractNote = {The ever–increasing demand for stationary energy storage has driven the prosperous investigation of low–cost sodium ion batteries. The inferior long–term cycling stability of cathode materials is a significant roadblock toward the wide commercialization of sodium ion batteries. This study enlightens a path toward empowering stable sodium ion batteries through incisive diagnostics of the multiscale surface chemical processes in layered oxide materials (e.g., O3–NaNi1/3Fe1/3Mn1/3O2). The major challenges are unraveled in a promising sodium layered cathode material using a range of complementary advanced spectroscopic and imaging diagnostic techniques. It is discovered that the cathode–electrolyte interfacial reaction triggers transition metal reduction, heterogeneous surface reconstruction, metal dissolution, and formation of intragranular nanocracks. These surface chemistry driven processes are partly responsible for significant performance decay. This diagnostic study also rationalizes the elemental substitution and surface passivation methods that are widely applied in the field. The prepassivated and Ti–substituted cathode materials allow for significantly improved cycling stability by inhibiting the metal dissolution. Furthermore, incisively diagnosing the interfacial chemistry not only creates scientific insights into understanding sodium cathode chemistry, but also represents an advance toward establishing universal interfacial design principles for all alkali metal ion cathode materials.},
doi = {10.1002/aenm.201801975},
journal = {Advanced Energy Materials},
issn = {1614-6832},
number = 34,
volume = 8,
place = {United States},
year = {2018},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on October 30, 2019
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