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Title: Structure–property insights into nanostructured electrodes for Li-ion batteries from local structural and diffusional probes

Microwave heating presents a faster, lower energy synthetic methodology for the realization of functional materials. Here, we demonstrate for the first time that employing this method also leads to a decrease in the occurrence of defects in olivine structured LiFe 1–xMn xPO 4. For example, the presence of antisite defects in this structure precludes Li + diffusion along the b-axis leading to a significant decrease in reversible capacities. Total scattering measurements, in combination with Li + diffusion studies using muon spin relaxation (μ+SR) spectroscopy, reveal that this synthetic method generates fewer defects in the nanostructures compared to traditional solvothermal routes. Our interest in developing these routes to mixed-metal phosphate LiFe 1–xMn xPO 4 olivines is due to the higher Mn 2+/ 3+ redox potential in comparison to the Fe 2+/ 3+ pair. Here, single-phase LiFe 1–xMn xPO 4 (x = 0, 0.25, 0.5, 0.75 and 1) olivines have been prepared following a microwave-assisted approach which allows for up to 4 times faster reaction times compared to traditional solvothermal methods. Interestingly, the resulting particle morphology is dependent on the Mn content. We also examine their electrochemical performance as active electrodes in Li-ion batteries. In conclusion, these results present microwave routes asmore » highly attractive for reproducible, gram-scale syntheses of high quality nanostructured electrodes which display close to theoretical capacity for the full iron phase.« less
Authors:
 [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [2] ;  [3] ; ORCiD logo [2] ;  [3] ; ORCiD logo [4] ; ORCiD logo [1]
  1. Univ. of Glasgow, Glasgow (United Kingdom)
  2. STFC Rutherford Appleton Lab., Didcot (United Kingdom)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
BNL-114789-2017-JA; BNL-203307-2018-JAAM
Journal ID: ISSN 2050-7488; R&D Project: PM011; KC0201060; TRN: US1800355
Grant/Contract Number:
SC0012704; SC00112704
Type:
Published Article
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
OSTI Identifier:
1411284
Alternate Identifier(s):
OSTI ID: 1412774; OSTI ID: 1425094