Lithium–sulfur batteries are
one of the most promising next
generation electrochemical devices with low cost and high energy density.
Up to now, various metal oxides with strong interaction with lithium
polysulfides (LiPs) have been designed as sulfur hosts to inhibit
the notorious shuttle effect. Nitrogen doping on metal oxides can
not only improve their shortcomings of poor electrical conductivity,
but also introduce additional oxygen vacancies to further enhance
their interaction with LiPs. In this work, the nitrogen-doped titanium
monoxide (N–TiO) nanospheres have been first synthesized through
a one-step method based on the synergistic effect of carbothermal
reduction and nitridation reaction. The X-ray diffraction results
suggested the gradually changed diffraction peak position, corresponding
to the nitridation process. Through the calculation of Gibbs free
energies in the temperature range of 800–1500 K, it was confirmed
that TiO2 can directly transform to TiO and then to TiN.
Moreover, the structural characterization and X-ray photoelectron
spectroscopy results suggested the synthesized N–TiO nanospheres
contain mixed valences of Ti4+, Ti3+, and Ti2+, together with a significantly increased O vacancy concentration.
By using N–TiO/S as the cathode, a high initial capacitance
of 1438 mA h g–1 at 0.2 C can be achieved, which
was higher than those of the undoped TiO/S and TiN/S electrodes. In
addition, such a cathode also delivered an initial discharge capacity
of 1105 mA h g–1 at 2 C, and retained 474 mA h g–1 after 800 cycles, corresponding to the capacity decay
rate of 0.071% per cycle. The strong interaction between O vacancies
in N–TiO and LiPs, which has been confirmed through visible
adsorption experiment and cyclic voltammetry curves of the Li2S6 symmetric cells, is the main reason for its
excellent electrochemical performance. This work can provide new ideas
for the preparation and application of N-doped metal oxide materials
in the field of lithium–sulfur batteries.