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Title: Phase evolution of conversion-type electrode for lithium ion batteries

Journal Article · · Nature Communications
 [1];  [1];  [2];  [3]; ORCiD logo [4];  [5];  [6];  [5];  [6];  [4]; ORCiD logo [7];  [5]; ORCiD logo [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Centre for Functional Nanomaterials
  2. Argonne National Lab. (ANL), Argonne, IL (United States). X-Ray Science Division. Advanced Photon Source; China Univ. of Petroleum, Beijing (China). Dept. of Materials Science and Engineering
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Centre for Functional Nanomaterials; Univ. of Waterloo, ON (Canada). Dept. of Chemical Engineering. Waterloo Inst. for Nanotechnology. Waterloo Inst. for Sustainable Energy
  4. Univ. of Waterloo, ON (Canada). Dept. of Chemical Engineering. Waterloo Inst. for Nanotechnology. Waterloo Inst. for Sustainable Energy
  5. Argonne National Lab. (ANL), Argonne, IL (United States). X-Ray Science Division. Advanced Photon Source
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Dept.
  7. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Materials Science and Engineering

Batteries with conversion-type electrodes exhibit higher energy storage density but suffer much severer capacity fading than those with the intercalation-type electrodes. The capacity fading has been considered as the result of contact failure between the active material and the current collector, or the breakdown of solid electrolyte interphase layer. Here, using a combination of synchrotron X-ray absorption spectroscopy and in situ transmission electron microscopy, we investigate the capacity fading issue of conversion-type materials by studying phase evolution of iron oxide composited structure during later-stage cycles, which is found completely different from its initial lithiation. The accumulative internal passivation phase and the surface layer over cycling enforce a rate-limiting diffusion barrier for the electron transport, which is responsible for the capacity degradation and poor rate capability. This work directly links the performance with the microscopic phase evolution in cycled electrode materials and provides insights into designing conversion-type electrode materials for applications.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC); Natural Sciences and Engineering Research Council of Canada (NSERC)
Grant/Contract Number:
AC02-06CH11357; SC0012704
OSTI ID:
1542127
Alternate ID(s):
OSTI ID: 1515155
Report Number(s):
BNL-211691-2019-JAAM; 151599
Journal Information:
Nature Communications, Vol. 10; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 73 works
Citation information provided by
Web of Science

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