Journal
JOURNAL OF POWER SOURCES
Volume 283, Issue -, Pages 423-428Publisher
ELSEVIER
DOI: 10.1016/j.jpowsour.2015.02.087
Keywords
Lithium rich; Structural transformation; Spinel; High-energy-density lithium-ion batteries; Magnetic frustration
Funding
- U.S. Department of Energy (DOE) [DE-AC05-00OR22725]
- DOE Energy Efficiency and Renewable Energy (EERE)
- Vehicle Technologies Office (VTO)
- Applied Battery Research (ABR) Program
- DOE Basic Energy Sciences (BES), Materials Sciences and Engineering Division
- VTO's ABR Program
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Making all-electric vehicles (EVs) commonplace in transportation applications will require affordable high-power and high-energy-density lithium-ion batteries (LIBs). The quest for suitable cathode materials to meet this end has currently plateaued with the discovery of high-voltage (>= 4.7 V vs. Li+), high capacity (similar to 250 mAh/g) lithium manganese-rich (LMR) layered composite oxides. Despite the promise of LMR oxides in high-energy-density LIBs, an irreversible structural change has been identified in this work that is governed by the formation of a 'permanent' spin-glass type magnetically frustrated phase indicating a dominant AB(2)O(4) (A = Li, B = Mn) type spinel after a short-term lithium deintercalation (charging) and intercalation (discharging) process. Furthermore, reduction of transition metal (Mn) ions from the 4+ state (pristine LMR) to 3+ (cycled LMR), which alters the intercalation redox chemistry and suggests the presence of 'unfilled' lithium vacancies and/or oxygen vacancies in the lattice after cycling, has presented a major stumbling block. These situations result in both loss of capacity and fading of the voltage profile, and these combined effects significantly reduce the high energy density over even short-term cycling. (C) 2015 Elsevier B.V. All rights reserved.
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