Ionic Liquid-Assisted Synthesis of Higher Loaded Ni/Fe Dual-Atom Catalysts in N, F, B Codoped Carbon Matrix for Accelerated Sulfur Reduction Reaction

In response to mitigating the severe shuttle effect within lithium-sulfur batteries, single-atom catalysts have emerged as one of the most effective solutions. Here, N, F, B codoped porous hollow carbon nanocages (NFB-NiFe@NC) with high Ni and Fe doping are rationally designed and synthesized using ionic liquids (ILs) as dopants. The introduction of ILs inhibits the growth of zeolitic imidazolate framework-8 (ZIF8), resulting in NFB-ZIF8 precursors with smaller particle sizes, enabling higher loading dual-atom catalysts. Meanwhile, the abundant heteroatoms increase the reactive sites and alter the carbon matrix's nonpolar intrinsic properties, thus enhancing the chemisorption of polysulfides. The synergistic interaction of the heteroatoms with Ni and Fe dual-atoms ultimately promotes the catalytic conversion kinetics of polysulfides. As a result of these beneficial properties, the cells prepared using the NFB-NiFe@NC modified separator exhibit significantly improved performance, including a high initial capacity of 1448 mAh g-1 at 0.2 C. Even at a high S-loading of 7.6 mg cm-2, the ideal area capacity of 8.38 mAh cm-2 can still be maintained at 0.1 C. New insights are provided here for designing highly loaded dual-atom catalysts for application in lithium-sulfur batteries. N, F, and B co-doped Ni and Fe diatomic catalysts (NFB-NiFe@NC) can effectively enhance the redox kinetics and suppress the shuttle effect in lithium-sulfur batteries. The cells assembled with NFB-NiFe@NC modified separators can still maintain an ideal area capacity of 8.38 mAh cm-2 at 0.1 C even under the high S loading condition of 7.6 mg cm-2. image