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Insights into the Enhanced Cycle and Rate Performances of the F-Substituted P2-Type Oxide Cathodes for Sodium-Ion Batteries

Journal Article · · Advanced Energy Materials
 [1];  [2];  [3];  [4];  [5];  [6];  [3];  [3];  [3];  [3];  [3];  [7];  [3];  [3];  [8]
  1. Tianjin Univ. (China). School of Chemical Engineering and Technology; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States)
  2. Univ. of Pittsburgh, PA (United States). Dept. of Electrical and Computer Engineering
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy and Transportation Science Division
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Juelich Center for Neutron Science, Outstation at the Spallation Neutron Source
  6. Ames Lab., and Iowa State Univ., Ames, IA (United States)
  7. Tianjin Univ. (China). School of Chemical Engineering and Technology
  8. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States)
+ Show Author Affiliations
A series of F-substituted Na2/3Ni1/3Mn2/3O2-xFx (x = 0, 0.03, 0.05, 0.07) cathode materials have been synthesized and characterized by solid-state 19F and 23Na NMR, X-ray photoelectron spectroscopy, and neutron diffraction. The underlying charge compensation mechanism is systematically unraveled by X-ray absorption spectroscopy and electron energy loss spectroscopy (EELS) techniques, revealing partial reduction from Mn4+ to Mn3+ upon F-substitution. It is revealed that not only Ni but also Mn participates in the redox reaction process, which is confirmed for the first time by EELS techniques, contributing to an increase in discharge specific capacity. The detailed structural transformations are also revealed by operando X-ray diffraction experiments during the intercalation and deintercalation process of Na+, demonstrating that the biphasic reaction is obviously suppressed in the low voltage region via F-substitution. Hence, the optimized sample with 0.05 mol f.u.-1 fluorine substitution delivers an ultrahigh specific capacity of 61 mAh g-1 at 10 C after 2000 cycles at 30 °C, an extraordinary cycling stability with a capacity retention of 75.6% after 2000 cycles at 10 C and 55 °C, an outstanding full battery performance with 89.5% capacity retention after 300 cycles at 1 C. This research provides a crucial understanding of the influence of F-substitution on the crystal structure of the P2-type materials and opens a new avenue for sodium-ion batteries.
Research Organization:
Ames Laboratory (AMES), Ames, IA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-06CH11357; AC02-07CH11358; AC05-00OR22725
OSTI ID:
1608689
Alternate ID(s):
OSTI ID: 1808128
OSTI ID: 1607596
OSTI ID: 1630505
Report Number(s):
IS--J 10,187
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 19 Vol. 10; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

25 ENERGY STORAGE
F‐substitution
P2‐type oxide
charge compensation mechanism
long cycle stability
sodium battery