Sulfur hosts with rationally designed chemistry to confine and convert lithium polysulfides are of prime importance for high-performance lithium-sulfur batteries. A molten salt electrochemical modulation of iron-carbon-nitrogen is herein demonstrated as formation of hollow nitrogen-doped carbon with grafted Fe 3 C nanoparticles (Fe 3 C@C@Fe 3 C), which is rationalized as an excellent sulfur host for lithiumsulfur batteries. Fe 3 C over nitrogen-doped carbon contributes to enhanced adsorption and catalytic conversion of lithium polysulfides. The sulfur-loaded Fe 3 C@C@Fe 3 C electrodes hence show a high capacity, good cyclic stability, and enhanced rate performance. This work highlights the unique chemistry of metal carbides on facilitating adsorption-conversion process of lithium polysulfides, and also extends the scope of molten salt electrolysis to elaboration of energy materials.
Electrochemicalenergystorageisakey-enablingprotocoltoachieve a carbon-neutral world. Lithium-sulfur (Li-S) batteries hold great promise to upgrade lithium-ion batteries (LIBs) because of high energy density, low cost and environmental benignity. [1,2] Setbacks in large-scale application of Li-S batteries include intrinsically low conductivity of sulfur and lithium sulfide (Li 2 S), shuttling effects caused by dissolution of lithium polysulfides (LiPSs), and tardy conversion kinetics of LiPSs. [3][4][5][6] The aforenamed challenges can effectively be ameliorated by constructing sulfur hosts with hollow structures and specific compositions. [7,8] Hollow structure could physically lock LiPSs within confined spaces and hence restrain shuttling between electrodes. [9] Sulfur/nanostructured carbon composites could greatly improve conductivity and cycling ability. [8] Other sulfur hosts were introduced to improve the adsorption of LiPSs, including metals, [10] metal carbides, [10,11] oxides, [12] nitrides, [13,14] sulfides and metal-free mediators. [15] Metal carbides are intriguing due to strong adsorption of LiPSs over the high-polarity surface and catalytic conversion of LiPSs. The synergy between adsorption and catalytic conversion of metal carbides thus suppresses the inconvenient