4.6 Article

Introducing high-valence elements into cobalt-free layered cathodes for practical lithium-ion batteries

Journal

NATURE ENERGY
Volume 7, Issue 10, Pages 946-954

Publisher

NATURE PORTFOLIO
DOI: 10.1038/s41560-022-01106-6

Keywords

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Funding

  1. Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant - Ministry of Trade, Industry and Energy of the Korean government [20214000000320]
  2. National Research Foundation of Korea (NRF) - Korea government Ministry of Education and Science Technology (MEST) [NRF-2018R1A2B3008794]
  3. Korea Institute of Energy Technology Evaluation & Planning (KETEP) [20214000000320] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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Eliminating cobalt from nickel-rich layered cathodes is crucial for reducing material cost and promoting sustainable development of Li-ion batteries. By adding 1 mol% molybdenum, the Li(Ni0.89Mn0.1Mo0.01)O-2 cathode exhibits improved performance in terms of capacity and cycling stability, thanks to grain size refinement and enhanced cation ordering.
The elimination of Co from Ni-rich layered cathodes is considered a priority to reduce their material cost and for sustainable development of Li-ion batteries (LIBs) as Co is becoming increasingly scarce. The introduction of 1 mol% Mo into Li(Ni0.9Mn0.1) O-2 delivers 234 mAh g(-1) at 4.4V. The cycling stability of a full cell featuring the Li(Ni0.89Mn0.1Mo0.01)O-2 (Mo-NM90) cathode is enhanced with a modified electrolyte; retaining 86% of its initial capacity after 1,000 cycles while providing 880 Wh kg(cathode)(-1). The grain size refinement achieved by Mo doping dissipates the deleterious strain from abrupt lattice contraction through fracture toughening and the removal of local compositional inhomogeneities. Enhanced cation ordering induced by the presence of Mo6+ also stabilizes the delithiated structure through a pillar effect. The Mo-NM90 cathode is able to deliver a high capacity with cycling stability suitable for the long service life for electric vehicles at a reduced material cost, furthering the realization of a commercially viable Co-free cathode for LIBs.

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