Conductive Al-Doped ZnO Framework Embedded with Catalytic Nanocages as a Multistage-Porous Sulfur Host in Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries possess many practical challenges including the lithium polysulfide (LiPS) “shuttle effect” and their sluggish conversion kinetics. To address these issues, a unique hierarchical porous architecture, combining highly conductive ordered macroporous skeleton and embedded microporous particles is rationally designed as a dual-effective polysulfide immobilizer and conversion promoter. In this nanoporous architecture, Al-doped ZnO (AZO) acts as a conductive macroporous framework, profiting chemical anchoring of LiPS as well as facilitating electrolyte infiltration and ion diffusion; Co nanoparticle-anchored N-doped carbon (Co-NC) derived from CoZn-metal–organic framework is embedded in the macropores to further strengthen the LiPS adsorption, catalytically accelerating conversion kinetics of LiPS simultaneously. Consequently, the Co-NC@AZO/S cathode delivers a notable rate capability of 635.5 mA h g–1 at 5 C. A high area capacity of about 5.8 mA h cm–2 with a mass loading of 6.8 mg cm–2 is also achieved under a lean electrolyte (E/S = 5.7). Additionally, the Li–S pouch cells equipped with Co-NC@AZO can be extended to sulfur loading as high as 4.0 mg cm–2, delivering a superb capability of 897.5 mA h g–1 after 100 cycles. This work puts forward a design for stably cycled and practically viable Li–S batteries.