Journal
ENERGY & ENVIRONMENTAL SCIENCE
Volume 4, Issue 12, Pages 4978-4983Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c1ee02283k
Keywords
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Funding
- National Research Foundation [NRF-2010-C1AAA001-0029018]
- Converging Research Center [2011K000600, 2011K000974]
- Ministry of Knowledge Economy [10037918]
- US National Science Foundation [ECCS 1002282]
- Fundamental R&D Program for Technology of World Premier Materials
- Korea Evaluation Institute of Industrial Technology (KEIT) [10037918] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Controlling the crystallographic structure in olivine lithium phosphates is crucial for obtaining superior electronic (J. Electrochem. Soc., 2002, 149, A1184-A1189) and ionic conductivities (Electrochem. Solid-State Lett., 2006, 9, A352-A355; Electrochem. Solid-State Lett., 2006, 9, A439-A442; Nat. Mater., 2002, 1, 123-128), and stability, for use as cathodes in lithium batteries. Here, we report a completely new approach to enhance Li+ extraction and transport in LiCoPO4 through Fe doping. We show that preferential Fe occupation of the 4c sites suppresses 4a-4c antisite mixing of Li and Co, thereby stabilizing the olivine structure by compensating for the Co-encapsulating oxygen octahedron shrinkage due to Co2+ oxidation during Li+ extraction. The structural stabilization gives rise to similar to 10% higher charge capacity at a two-fold lower resistance than the undoped counterparts besides accelerating the intercalation/extraction kinetics. Our findings provide key atomistic-level insights that pave the way for the rational design and realization of new types of metal-doped cathode materials for lithium batteries and related applications.
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