Lithium–sulfur
(Li–S) batteries are severely hindered
by the low sulfur utilization and short cycling life, especially at
high rates. One of the effective solutions to address these problems
is to improve the sulfiphilicity of lithium polysulfides (LiPSs) and
the lithiophilicity of the lithium anode. However, it is a great challenge
to simultaneously optimize both aspects. Herein, by incorporating
the merits of strong absorbability and high conductivity of SnS with
good catalytic capability of ZnS, a ZnS-SnS heterojunction coated
with a polydopamine-derived N-doped carbon shell (denoted as ZnS-SnS@NC)
with uniform cubic morphology was obtained and compared with the ZnS-SnS2@NC heterostructure and its single-component counterparts
(SnS@NC and SnS2@NC). Theoretical calculations, ex situ XANES, and in situ Raman spectrum
were utilized to elucidate rapid anchoring-diffusion-transformation
of LiPSs, inhibition of the shuttling effect, and improvement of the
sulfur electrochemistry of bimetal ZnS-SnS heterostructure at the
molecular level. When applied as a modification layer coated on the
separator, the ZnS-SnS@NC-based cell with optimized lithiophilicity
and sulfiphilicity enables desirable sulfur electrochemistry, including
high reversibility of 1149 mAh g–1 for 300 cycles
at 0.2 C, high rate performance of 661 mAh g–1 at
10 C, and long cycle life with a low fading rate of 0.0126% each cycle
after 2000 cycles at 4 C. Furthermore, a favorable areal capacity
of 8.27 mAh cm–2 is maintained under high sulfur
mass loading of 10.3 mg cm–2. This work furnishes
a feasible scheme to the rational design of bimetal sulfides heterostructures
and boosts the development of other electrochemical applications.