High specific capacity and long cycle
life are the key to high-performance
lithium–sulfur (Li–S) batteries, but they are hard to
achieve simultaneously due to the notorious polysulfide shuttle effect.
Transition metal oxide nanocatalysts are expected to help address
the above issue, but their low conductivity and cumbersome synthesis
process limit their application. Here, we propose a defect engineering
strategy to induce electron rearrangement by heteroatom doping. Boron-doped
spinel-type oxide (B-ZnCo2O4‑x) is synthesized
by a two-step hydrothermal method for separator modification. The
boron-produced oxygen vacancy (OV) increases unsaturated
sites by changing the electron cloud density, and therefore, the B-ZnCo2O4‑x nanocatalyst can reduce the reaction
energy barrier and accelerate the nucleation and activation rate of
Li2S. Meanwhile, the unique pore defects effectively increase
the Li+ flux and ensure battery performance at a high rate
and high sulfur loading. The battery equipped with a B-ZnCo2O4‑x-modified separator delivered an initial specific
capacity of 1108 mAh g–1 at 0.2 C and a capacity
retention rate of 80.4% at 0.5 C after 200 cycles. In particular,
at a high sulfur loading of 10.0 mg cm–2, the battery
yielded a first-cycle capacity of 1321.9 mAh g–1. This work demonstrates that boron-doping-enabled defect engineering
is an effective strategy to improve the catalytic activity of transition
metal oxides for application in Li–S batteries.