Cobalt-free
layered oxides have emerged as promising candidates
for next-generation cathodes for lithium-ion batteries. However, implementation
of these materials has been hindered by their low rate capability,
structural instability, and rapid capacity decay during cycling. Recent
studies have shown that introducing cation dopants into layered oxides
can strongly improve their electrochemical properties, but the underlying
atomic-scale mechanisms remain elusive. In this work, we use a combination
of atomic-resolution scanning transmission electron microscopy and
first-principle calculations to reveal the microscopic origin of enhanced
electrochemical properties in LiNi0.5Mn0.5O2 doped with ∼1 atom % Mo. Our results indicate that
the Mo dopant hinders Li+/Ni2+ cation mixing
and suppresses detrimental phase transformations near the particle
surface and at intragranular grain boundaries, which enhances the
cathode’s reversible capacity and cycling stability. Overall,
this work provides important insights on how cation doping affects
the structure and electrochemical properties of layered oxide cathodes.
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