Manganese-based compounds are expected
to become promising candidates
for lithium-ion battery anodes by virtue of their high theoretical
specific capacity and low conversion potential. However, their application
is hindered by their inferior electrical conductivity and drastic
volume variations. In this work, a unique heterostructure composed
of MnO and MnS spatially confined in pyrolytic carbon microspheres
(MnO@MnS/C) was synthesized through an integrated solvothermal method,
calcination, and low-temperature vulcanization technology. In this
architecture, heterostructured MnO@MnS nanoparticles (∼10 nm)
are uniformly embedded into the carbonaceous microsphere matrix to
maintain the structural stability of the composite. Benefiting from
the combination of structural and compositional features, the MnO@MnS/C
enables abundance in electrochemically active sites, alleviated volumetric
variation, a rich conductive network, and enhanced lithium-ion diffusion
kinetics, thus yielding remarkable rate capability (1235 mAh·g–1 at 0.2 A·g–1 and 608 mAh·g–1 at 3.2 A·g–1) and exceptional
cycling stability (522 mAh·g–1 after 2000 cycles
at 3.0 A·g–1) as a competitive anode material
for lithium-ion batteries. Density functional theory calculations
unveil that the heterostructure promotes the transfer of electrons
with improved conductivity and also accelerates the migration of lithium
ions with reduced polarization resistance. This combined with the
enhancement brought by spatial confinement endows the MnO@MnS/C with
remarkable lithium storage performance.