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For lithium‐sulfur batteries (Li‐S batteries), a high‐content electrolyte typically can exacerbate the shuttle effect, while a lean electrolyte may lead to decreased Li‐ion conductivity and reduced catalytic conversion efficiency, so achieving an appropriate electrolyte‐to‐sulfur ratio (E/S ratio) is essential for improving the battery cycling efficiency. A quasi‐solid electrolyte (COF‐SH@PVDF‐HFP) with strong adsorption and high catalytic conversion was constructed for in situ covalent organic framework (COF) growth on highly polarized polyvinylidene fluoride‐hexafluoropropylene (PVDF‐HFP) fibers. COF‐SH@PVDF‐HFP enables efficient Li‐ion conductivity with low‐content liquid electrolyte and effectively suppresses the shuttle effect. The results based on in situ Fourier‐transform infrared, in situ Raman, UV–Vis, X‐ray photoelectron, and density functional theory calculations confirmed the high catalytic conversion of COF‐SH layer containing sulfhydryl and imine groups for the lithium polysulfides. Lithium plating/stripping tests based on Li/COF‐SH@PVDF‐HFP/Li show excellent lithium compatibility (5 mAh cm−2 for 1400 h). The assembled Li‐S battery exhibits excellent rate (2 C 688.7 mAh g−1) and cycle performance (at 2 C of 568.8 mAh g−1 with a capacity retention of 77.3% after 800 cycles). This is the first report to improve the cycling stability of quasi‐solid‐state Li‐S batteries by reducing both the E/S ratio and the designing strategy of sulfhydryl‐functionalized COF for quasi‐solid electrolytes. This process opens up the possibility of the high performance of solid‐state Li‐S batteries. The sulfhydryl‐covalent organic framework functionalized polyvinylidene fluoride‐hexafluoropropylene as a quasi‐solid electrolyte enhances the chemical affinity of polysulfides in lithium‐sulfur batteries, accelerating the conversion reaction kinetics, improving the catalytic conversion efficiency of polysulfides and the utilization rate of active materials in lithium‐sulfur batteries, and providing a potential reference for the electrolyte design of high‐loading and high‐performance lithium‐sulfur batteries.

Low electrolyte/sulfur ratio (E/S) is an important factor in increasing the energy density of lithium-sulfur batteries (LSBs). Recently, the E/S has been widely lowered using catalytic hosts that can suppress “shuttle effect” during cycling by relying on a limited adsorption area. However, the shelf-lives of these cathodes have not yet received attention. Herein, we show that the self-discharge of sulfur cathodes based on frequently-used catalytic hosts is serious under low E/S because the “shuttle effect” during storage process caused by polysulfides (PSs) disproportionation cannot be suppressed using a limited adsorption area. We further prove that the adsorption strength toward PSs, which is unfortunately weak in commonly-used catalytic hosts, is critical for effectively hindering the disproportionation of the PSs. Subsequently, to verify this conclusion, we prepare a sulfur-doped titanium nitride (S-TiN) catalytic array host. As the adsorption strength and catalytic activity of TiN can be improved by S doping simultaneously, the constructed S/S-TiN cathodes under a low E/S (6.5 µL·mg −1 ) exhibit better shelf-life and cycle-stability than those of S/TiN cathodes. Our work suggests that enhancing the adsorption strength of catalytic hosts, while maintaining their function to reduce E/S, is crucial for practical LSBs.

Li-S batteries are considered as a highly promising candidate for the next-generation energy storage system, attributing to their tremendous energy density. However, the two-dimensional island nucleation-growth process of lithium sulfide leads to a thick insulating film covering the electrode, inducing slow electrons transfer and mass-transfer of ions and liquid sulfur species in working Li-S cells. Here, we demonstrate a bio-inspired strategy of constructing ant-nest-like hierarchical porous ultrathin carbon nanosheet networks with the implants of metallic nanoparticles electrocatalysts (HPC-MEC) as efficient nanoreactors enabling rapid mass transfer, via a simple and green NaCl template. Such nanoreactors with a large active surface area could effectively anchor polysulfides for mitigating the shuttle effect, facilitating uniformly thin Li 2 S film, and promoting the mass transfer for fast sulfur species conversions. This helps contribute to a continuously high sulfur utilization in Li-S batteries with the HPC-MEC reactors. As a typical exhibition, cobalt embedded hierarchical porous carbon (HPC-Co) could realize to deliver a remarkably high specific capacity of 1,540.6 mAh·g −1 , an excellent rate performance of 878.8 mAh·g −1 at 2 C, and high area capacity of 11.6 mAh·cm −2 at a high sulfur load of 10 mg·cm −2 and low electrolyte/sulfur ratio of 5 µL·mg −1 .