Lithium–sulfur batteries suffer from volume variation,
insulation
of sulfur, and a severe shuttle effect, leading to an inferior cycling
performance. Herein, a dual cross-linked binder (CPS), which contains
chemical covalent bonds and physical hydrogen bonds, is fabricated
for lithium–sulfur batteries through carboxymethyl cellulose
conjugated with catechol groups and thiolated branched polyethylenimine.
The chemical covalent cross-linked bonds are formed via the Michael
addition reaction that avoids consumption of catechol groups. The
dynamic hydrogen bonds consume the stress energy and repair the cracks,
which are caused by the remarkable volume change of sulfur. Combining
the rigid and soft moieties, polar groups, and dual cross-linked structure
in the CPS, the CPS prominently tolerates and buffers the huge volume
change of active materials, resulting in maintenance of the cathode
integrity. Additionally, the CPS effectively immobilizes the lithium
polysulfides into the cathodes, remarkably accelerates the reaction
kinetics, and significantly facilitates lithium-ion diffusion. As
a result, the sulfur cathode with CPS exhibits a high initial capacity
of 1380 mAh g–1. At a mass loading of 8.5 mg cm–2 and an electrolyte/sulfur ratio of 5 μL mg–1, the sulfur cathode with CPS retains 627 mAh g–1 after 100 cycles at a rate of 0.5 C.