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Title: Three-dimensional localization of nanoscale battery reactions using soft X-ray tomography

Battery function is determined by the efficiency and reversibility of the electrochemical phase transformations at solid electrodes. The microscopic tools available to study the chemical states of matter with the required spatial resolution and chemical specificity are intrinsically limited when studying complex architectures by their reliance on two-dimensional projections of thick material. Here in this paper, we report the development of soft X-ray ptychographic tomography, which resolves chemical states in three dimensions at 11 nm spatial resolution. We study an ensemble of nano-plates of lithium iron phosphate extracted from a battery electrode at 50% state of charge. Using a set of nanoscale tomograms, we quantify the electrochemical state and resolve phase boundaries throughout the volume of individual nanoparticles. These observations reveal multiple reaction points, intra-particle heterogeneity, and size effects that highlight the importance of multi-dimensional analytical tools in providing novel insight to the design of the next generation of high-performance devices.
Authors:
 [1] ;  [2] ;  [3] ; ORCiD logo [4] ;  [5] ;  [6] ;  [2] ; ORCiD logo [2] ;  [2] ;  [7] ; ORCiD logo [8] ;  [9] ; ORCiD logo [2] ;  [2] ; ORCiD logo [8] ;  [2] ;  [2] ; ORCiD logo [10] ; ORCiD logo [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of Illinois, Chicago, IL (United States). Dept. of Chemistry
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  3. Univ. of Illinois, Chicago, IL (United States). Dept. of Chemistry; Chungnam National Univ., Daejeon (South Korea). Dept. of Materials Science and Engineering
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  5. Univ. of Cambridge (United Kingdom). Dept. of Chemistry; Stony Brook Univ., NY (United States). Dept. of Chemistry
  6. Univ. of Cambridge (United Kingdom). Dept. of Chemistry
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Engineering Division
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Computational Research Division
  9. Uppsala Univ. (Sweden). Dept. of Cell and Molecular Biology
  10. Univ. of Illinois, Chicago, IL (United States). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
AC02-76SF00515; AC02-05CH11231; SC0012583
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Research Foundation of Korea (NRF); USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR) (SC-21)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; Batteries; Imaging
OSTI Identifier:
1427169
Alternate Identifier(s):
OSTI ID: 1433136