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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


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