• 연구
  • 연구성과



Site-Specific Transition Metal Occupation in Multicomponent Pyrophosphate for Improved Electrochemical and Thermal Properties in Lithium Battery Cathodes: A Combined Experimental and Theoretical Study

Rana. A. Shakoor, Heejin Kim, Woosuk Cho, Soo Yeon Lim, Hannah Song, Jung Woo Lee, Jeung Ku Kang, Yong-Tae Kim, Yousung Jung, and Jang Wook Choi


J. Am. Chem. Soc., Article ASAP

DOI: 10.1021/ja3042228

Publication Date (Web): June 21, 2012

Copyright © 2012 American Chemical Society


As an attempt to develop lithium ion batteries with excellent performance, which is desirable for a variety of applications including mobile electronics, electrical vehicles, and utility grids, the battery community has continuously pursued cathode materials that function at higher potentials with efficient kinetics for lithium insertion and extraction. By employing both experimental and theoretical tools, herein we report multicomponent pyrophosphate (Li2MP2O7, M = Fe1/3Mn1/3Co1/3) cathode materials with novel and advantageous properties as compared to the single-component analogues and other multicomponent polyanions. Li2Fe1/3Mn1/3Co1/3P2O7 is formed on the basis of a solid solution among the three individual transition-metal-based pyrophosphates. The unique crystal structure of pyrophosphate and the first principles calculations show that different transition metals have a tendency to preferentially occupy either octahedral or pyramidal sites, and this site-specific transition metal occupation leads to significant improvements in various battery properties: a single-phase mode for Li insertion/extraction, improved cell potentials for Fe2+/Fe3+ (raised by 0.18 eV) and Co2+/Co3+ (lowered by 0.26 eV), and increased activity for Mn2+/Mn3+ with significantly reduced overpotential. We reveal that the favorable energy of transition metal mixing and the sequential redox reaction for each TM element with a sufficient redox gap is the underlying physical reason for the preferential single-phase mode of Li intercalation/deintercalation reaction in pyrophosphate, a general concept that can be applied to other multicomponent systems. Furthermore, an extremely small volume change of 0.7% between the fully charged and discharged states and the significantly enhanced thermal stability are observed for the present material, the effects unseen in previous multicomponent battery materials.

For further details: http://pubs.acs.org/doi/abs/10.1021/ja3042228


  1. [SCIENTIFIC REPORTS] 이정용 (2013) "Plasmonic Forward Scattering Effect in Organic Solar Cells: A Powerful Optical Engineering Method"

    Read More
  2. [Microscopy] Osamu Terasaki (2013) "A review of fine structures of nanoporous materials as evidenced by microscopic methods"

    Read More
  3. [Science] 최장욱, William A. Goddard, and J. Fraser Stoddart (2013) "A Radically Configurable Six-State Compound"

    Read More
  4. [Nature Communications] Cafer T. Yavuz & Ali Coskun (2013) "Unprecedented high-temperature CO2 selectivity in N2-phobic nanoporous covalent organic polymers"

    Read More
  5. [Science] Osamu Terasaki (2012) "Synthesis of Self-Pillared Zeolite Nanosheets by Repetitive Branching"

    Read More
  6. [Nature] Keiichi Miyasaka & Osamu Terasaki (2012) Dodecagonal tiling in mesoporous silica

    Read More
  7. [JACS] 최장욱 & 정유성 (2012) "Site-Specific Transition Metal Occupation in Multicomponent Pyrophosphate for Improved Electrochemical and Thermal Properties in Lithium Battery Cathodes:

    Read More
  8. [Chem Mater] 김희진 & 정유성 (2012) "Ab Initio Study of the Sodium Intercalation and Intermediate Phases in Na0.44MnO2 for Sodium-Ion Battery"

    Read More
  9. [JPC Lett] Tod Pascal, William Goddard, & 정유성 (2012) "Stability of Positively Charged Solutes in Water: A Transition from Hydrophobic to Hydrophilic"

    Read More
  10. [JPC Lett] 박준호 & 정유성 (2012) "Tuning Metal–Organic Frameworks with Open-Metal Sites and Its Origin for Enhancing CO2 Affinity by Metal Substitution"

    Read More
Board Pagination Prev 1 2 3 4 5 6 7 Next
/ 7