Graphdiyne-Based Heteronuclear Dual-Atom Catalysts Enable High-Energy-Density Lithium-Sulfur Batteries.

The practical application of lithium-sulfur (Li-S) batteries are hindered by lithium (Li) polysulfides (LiPSs) shuttling, sluggish sulfur (S) redox kinetics, and Li dendrite growth. Here, we report heteronuclear Co-Pt dual-atom catalysts (DACs) anchored on graphdiyne (GDY) (Co-Pt DAs/GDY) to boost S redox conversion kinetics and promote uniform Li deposition to enable high-energy-density Li-S batteries. The unique electronic coupling between sp-hybridized carbon of GDY and Co-Pt dual atoms triggers a p-d-d orbital resonance. This resonance optimizes the interfacial electronic configuration to promote strong d-p orbital hybridization with LiPSs, endowing dual-atom sites with site‑isolated redox‑complementary catalytic behavior toward sequential S redox reactions. Meanwhile, adjacent Pt atoms tailor Co sites to a high-spin state, further strengthening their adsorption and catalytic capabilities. Benefiting from these features, the redox kinetics and electrochemical performance of S cathodes are significantly enhanced, S@Co-Pt DAs/GDY cathodes deliver a remarkable areal capacity of 21.3 mA h cm-2 and an excellent cycling stability under realistic conditions. Moreover, Co-Pt DAs/GDY exhibits strong Li-ion affinity and offers dual-atom Li nucleation sites, enabling stable cycling of Li@Co-Pt DAs/GDY anodes for more than 9200 h. Assembled Ah-level Li-S pouch cells achieve a high-energy-density of 502 Wh kg-1 (based on the total cell mass).