Key Takeaways & Executive Findings
- •• Fe/Ni-N-PCNSs exhibit exceptional performance as a dual host for sulfur and lithium, achieving a record low capacity decay of 0.00025% per cycle over 1000 cycles in Li-S batteries. • The 2D porous structure and uniform Fe/Ni doping enable efficient polysulfide capture and fast redox kinetics, effectively suppressing the shuttle effect. • Enhanced lithiophilicity of the material promotes uniform lithium nucleation, preventing dendrite growth and enabling stable cycling over 850 hours in lithium metal batteries. • The template-free synthesis method offers a scalable and cost-effective approach for producing multifunctional carbon nanosheets for advanced energy storage.
Abstract
The major problem with lithium-sulfur (Li-S) batteries is their poor cycling stability because of slow redox kinetics in the cathode and the growth of lithium dendrites on the anode. We report the production of 2D porous carbon nanosheets doped with both Fe and Ni (Fe/Ni-N-PCNSs) by an easy and template-free approach that solve this problem. Because of their ultrathin porous 2D structure and uniform distribution of Fe and Ni dopants, they capture polysulfides, speed up the sulfur redox reaction, and improve the material's lithiophilicity, greatly suppressing the shuttling of polysulfides and dendrite growth on the lithium anode. As a result, it has an exceptional performance as a stable host for elemental sulfur and metallic lithium, producing a record long life of 1000 cycles with a very small capacity decay of 0.00025% per cycle in a Li-S battery and an excellent cycling stability of over 850 h with a small overpotential of >72 mV in a lithium metal battery. This work suggests the use of multifunctional-based 2D porous carbon nanosheets as a stable host for both elemental sulfur and metallic lithium to improve the Li-S battery performance.
1. Introduction
To satisfy the need for advanced energy storage, various novel storage systems have been developed. Lithium-sulfur (Li-S) batteries have been attracting a great deal of attention, owing to their theoretical specific energy (2500 Wh kg−1) and high theoretical specific capacity (1675 mAh g−1)[1–4]. Furthermore, there are numerous merits including low cost, natural abundance, and environmental friendliness that come with the usage of sulfur as an active material in the cathode. Therefore, Li-S batteries have become the most promising candidate for next-generation high energy density batteries. However, the commercialization of Li-S batteries is still impeded by a series of challenges, including dendrite growth in anode and continuous lithium polysulfide intermediates (Li2Sn, “4≤n≤8”) dissolution in electrolyte[5–8]. All these shortcomings result in poor safety, shorter cycle life, low Coulombic efficiency (CE), and low practical energy density. Hence, searching for effective ways to trap Li2Sn has been one of the key scientific issues for the practical application of Li-S batteries.
During the past decades, tremendous effort has been devoted to solving these issues for improving the performance of Li-S batteries. Physical confinement and chemical interaction are two main strategies to alleviate the “shuttle effect” of Li2Sn[9–10]. Due to high electronic conductivity, large surface area, and high stability, carbon materials have been widely applied in energy storage and conversation[11–12]. Carbon materials with various structures were also investigated for constructing the sulfur cathodes, including micro/mesoporous carbons[13], hollow carbon spheres[14], carbon nanotubes/nanofibers[15] and graphene[16]. For example, Geng et al. prepared 3D porous graphitic carbon composite embedded with sulfur nanoparticles (3DS@PGC) using an in-situ method[17]. As-synthesized 3D composite showed excellent cycling stability up to 1000 cycles at 2 C and accommodated as high as 90% (mass fraction) sulfur. Although carbon-based host materials with various nanostructures show superior electrical conductivity and a certain degree of physical confinement for sulfur, generally their surface characteristic is hydrophobic, which is not favorable for the adsorption of polysulfides during long-term cycling and lead to rapid capacity decay[18]. Therefore, to enhance the electrochemical performance of S/C composites and improve the interface interaction between ...
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Reddeppa Nadimicherla, TANG You-chen, LU Yu-heng, LIU Ru-liang (2025). Ultra-stable lithium-sulfur batteries using nitrogen-doped porous carbon nanosheets implanted with both Fe and Ni. SinoTechIntel Verified Research. https://doi.org/10.1016/S1872-5805(NCM2025-40-01-09)
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Frequently Asked Questions
What is the main problem with lithium-sulfur batteries addressed in this study?
The main problems are poor cycling stability due to slow redox kinetics in the cathode and lithium dendrite growth on the anode, which lead to the shuttle effect and safety issues.
How do Fe/Ni-N-PCNSs improve the performance of Li-S batteries?
Fe/Ni-N-PCNSs capture polysulfides, accelerate sulfur redox reactions, and enhance lithiophilicity, thereby suppressing the shuttle effect and dendrite growth, resulting in ultra-stable cycling.
What are the key performance metrics of the Fe/Ni-N-PCNSs in Li-S batteries?
The Fe/Ni-N-PCNSs achieve a record long life of 1000 cycles with a very small capacity decay of 0.00025% per cycle, and excellent cycling stability of over 850 hours with a small overpotential of >72 mV in lithium metal batteries.
What is the significance of the template-free synthesis method?
The template-free approach is easy and scalable, offering a cost-effective way to produce multifunctional 2D porous carbon nanosheets for advanced energy storage applications.
What are the potential applications of this material beyond Li-S batteries?
The material's dual functionality as a host for both sulfur and lithium suggests potential applications in other metal-sulfur batteries and lithium metal batteries, as well as in catalysis and energy storage devices.
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