skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Facile, ethylene glycol-promoted microwave-assisted solvothermal synthesis of high-performance LiCoPO 4 as a high-voltage cathode material for lithium-ion batteries

Abstract

Olivine-type LiCoPO 4 is considered a promising high-voltage cathode material for next-generation lithium-ion batteries. However, preparing high-performance LiCoPO 4 by a simple approach has been challenging. Herein, we present a facile and rapid (30 min) one-step microwave-assisted solvothermal synthesis route using a 1 : 1 (v/v) water/ethylene glycol (EG) binary solvent mixture and a temperature of 250 °C. Here, the technique delivers high-performance LiCoPO4nanoparticles without additional post-annealing or carbon coating steps. The as-prepared powder consists of single crystalline LiCoPO 4 and features a hexagonal platelet-like morphology with dimensions of 700-800 nm × 400-600 nm × 100-220 nm. Selected area electron diffraction (SAED) experiments reveal that the platelets show the smallest dimension along [010], which is the direction of the lithium diffusion pathways in the olivine crystal structure. Furthermore, the results indicate that the EG co-solvent plays an important role in tailoring the particle size, morphology, and crystal orientation of the material. Co L-edge soft X-ray absorption spectroscopy (XAS) of LiCoPO 4 are presented for the first time and confirm that the material only consists of Co 2+. Benefiting from the unique morphology, which facilitates Li-ion conduction, electrochemical measurements deliver an initial discharge capacity of 137 mA h g -1 atmore » 0.1 C, a remarkably stable capacity retention of 68% after 100 cycles at 0.5 C, and a specific energy density of 658 W h kg -1 based on its capacity and voltage, which is the best performance of LiCoPO 4 obtained from microwave-assisted solvothermal synthesis to date.« less

Authors:
 [1];  [1];  [1];  [2];  [3];  [4];  [1];  [1]
  1. Technical University of Munich, Garching (Germany)
  2. BMW AG, München (Germany)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1532177
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
RSC Advances
Additional Journal Information:
Journal Volume: 6; Journal Issue: 86; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ludwig, Jennifer, Marino, Cyril, Haering, Dominik, Stinner, Christoph, Nordlund, Dennis, Doeff, Marca M., Gasteiger, Hubert A., and Nilges, Tom. Facile, ethylene glycol-promoted microwave-assisted solvothermal synthesis of high-performance LiCoPO4 as a high-voltage cathode material for lithium-ion batteries. United States: N. p., 2016. Web. doi:10.1039/c6ra19767a.
Ludwig, Jennifer, Marino, Cyril, Haering, Dominik, Stinner, Christoph, Nordlund, Dennis, Doeff, Marca M., Gasteiger, Hubert A., & Nilges, Tom. Facile, ethylene glycol-promoted microwave-assisted solvothermal synthesis of high-performance LiCoPO4 as a high-voltage cathode material for lithium-ion batteries. United States. doi:10.1039/c6ra19767a.
Ludwig, Jennifer, Marino, Cyril, Haering, Dominik, Stinner, Christoph, Nordlund, Dennis, Doeff, Marca M., Gasteiger, Hubert A., and Nilges, Tom. Thu . "Facile, ethylene glycol-promoted microwave-assisted solvothermal synthesis of high-performance LiCoPO4 as a high-voltage cathode material for lithium-ion batteries". United States. doi:10.1039/c6ra19767a. https://www.osti.gov/servlets/purl/1532177.
@article{osti_1532177,
title = {Facile, ethylene glycol-promoted microwave-assisted solvothermal synthesis of high-performance LiCoPO4 as a high-voltage cathode material for lithium-ion batteries},
author = {Ludwig, Jennifer and Marino, Cyril and Haering, Dominik and Stinner, Christoph and Nordlund, Dennis and Doeff, Marca M. and Gasteiger, Hubert A. and Nilges, Tom},
abstractNote = {Olivine-type LiCoPO4 is considered a promising high-voltage cathode material for next-generation lithium-ion batteries. However, preparing high-performance LiCoPO4 by a simple approach has been challenging. Herein, we present a facile and rapid (30 min) one-step microwave-assisted solvothermal synthesis route using a 1 : 1 (v/v) water/ethylene glycol (EG) binary solvent mixture and a temperature of 250 °C. Here, the technique delivers high-performance LiCoPO4nanoparticles without additional post-annealing or carbon coating steps. The as-prepared powder consists of single crystalline LiCoPO4 and features a hexagonal platelet-like morphology with dimensions of 700-800 nm × 400-600 nm × 100-220 nm. Selected area electron diffraction (SAED) experiments reveal that the platelets show the smallest dimension along [010], which is the direction of the lithium diffusion pathways in the olivine crystal structure. Furthermore, the results indicate that the EG co-solvent plays an important role in tailoring the particle size, morphology, and crystal orientation of the material. Co L-edge soft X-ray absorption spectroscopy (XAS) of LiCoPO4 are presented for the first time and confirm that the material only consists of Co2+. Benefiting from the unique morphology, which facilitates Li-ion conduction, electrochemical measurements deliver an initial discharge capacity of 137 mA h g-1 at 0.1 C, a remarkably stable capacity retention of 68% after 100 cycles at 0.5 C, and a specific energy density of 658 W h kg-1 based on its capacity and voltage, which is the best performance of LiCoPO4 obtained from microwave-assisted solvothermal synthesis to date.},
doi = {10.1039/c6ra19767a},
journal = {RSC Advances},
number = 86,
volume = 6,
place = {United States},
year = {2016},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 14 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Issues and challenges facing rechargeable lithium batteries
journal, November 2001

  • Tarascon, J.-M.; Armand, M.
  • Nature, Vol. 414, Issue 6861, p. 359-367
  • DOI: 10.1038/35104644

Electronically conductive phospho-olivines as lithium storage electrodes
journal, September 2002

  • Chung, Sung-Yoon; Bloking, Jason T.; Chiang, Yet-Ming
  • Nature Materials, Vol. 1, Issue 2, p. 123-128
  • DOI: 10.1038/nmat732

Battery materials for ultrafast charging and discharging
journal, March 2009

  • Kang, Byoungwoo; Ceder, Gerbrand
  • Nature, Vol. 458, Issue 7235, p. 190-193
  • DOI: 10.1038/nature07853

Phospho-olivines as Positive-Electrode Materials for Rechargeable Lithium Batteries
journal, April 1997

  • Padhi, A. K.
  • Journal of The Electrochemical Society, Vol. 144, Issue 4, p. 1188-1194
  • DOI: 10.1149/1.1837571

One-Pot Microwave-Hydrothermal Synthesis and Characterization of Carbon-Coated LiMPO4 (M=Mn, Fe, and Co) Cathodes
journal, January 2009

  • Vadivel Murugan, A.; Muraliganth, T.; Manthiram, A.
  • Journal of The Electrochemical Society, Vol. 156, Issue 2, p. A79-A83
  • DOI: 10.1149/1.3028304