Key Takeaways & Executive Findings
- •• • FeNi3/CNS electrocatalyst delivers a rate capability of 852 mAh g−1 at 3.0 C, demonstrating superior high-rate performance for Li–S batteries. • • Long-term cycling stability is achieved with 639 mAh g−1 retained after 500 cycles at 1.0 C, indicating excellent capacity retention for practical applications. • • The catalyst enables stable operation across a wide temperature range from −15°C to 60°C, addressing performance degradation under extreme thermal conditions. • • A maximum areal capacity of 5.60 mAh cm−2 is attained at a sulfur loading of ~4.0 mg cm−2, meeting the requirements for high-energy-density batteries.
Abstract
High energy-density lithium–sulfur (Li–S) batteries with rapid intermediate conversion and forbidden shuttle effect require superior electrocatalysts with tunable catalytic activity. In this protocol, binary FeNi3 alloy nanoparticles homogeneously embedded within carbon nanosheets (FeNi3/CNS) are synthesized to regulate the conversions of sulfur species. Time of flight-secondary mass ion spectroscopy reveals a significantly improved catalytic effect of binary FeNi3 alloy compared to bare Ni, which is confirmed by a larger Li2S amount generated during in situ X-ray diffraction measurement. Further anode characterization validates efficient shuttling suppression and good lithium metal protection. In Li–S batteries, electrochemical tests demonstrate a remarkable rate capability of 852 mAh g−1 at 3.0 C, and outstanding long-term cycle at 1.0 C (639 mAh g−1 after 500 cycles). Even under a wide operation temperature range (−15–60 °C), Li–S batteries exhibit stable cycling with high specific capacities under high current rates. Moreover, Li–S batteries using FeNi3/CNS attain a maximum areal capacity of 5.60 mAh cm−2 under ~4.0 mg cm−2 sulfur. This study highlights the advantages of adopting binary or multi-component metal alloys as electrocatalysts and points out the research directions to advance Li–S batteries into practical applications.
1. Introduction
Lithium–sulfur (Li–S) batteries are a leading candidate for next-generation energy storage due to their high theoretical energy density and low cost of sulfur. However, their commercial viability is hindered by sluggish polysulfide conversion kinetics and the detrimental shuttle effect, which cause rapid capacity fade and poor rate capability. These issues are exacerbated under extreme temperatures: low temperatures increase electrolyte viscosity and slow ion transport, while high temperatures intensify polysulfide shuttling, leading to accelerated capacity loss. Conventional electrocatalysts, such as metal compounds and metal-organic frameworks, have been explored to mitigate these problems, but they often suffer from insufficient catalytic activity or poor stability under demanding operating conditions.
This study introduces binary FeNi3 alloy nanoparticles embedded in carbon nanosheets (FeNi3/CNS) as an advanced electrocatalyst for Li–S batteries. The binary alloy design leverages the synergistic interaction between Fe and Ni atoms to enhance catalytic activity toward polysulfide conversion, as evidenced by increased Li2S precipitation and suppressed shuttling. The material demonstrates exceptional rate capability (852 mAh g−1 at 3.0 C) and long-term cycling stability (639 mAh g−1 after 500 cycles at 1.0 C), while maintaining high performance across a wide temperature range (−15 to 60°C). These results underscore the potential of binary metal alloys to overcome the kinetic and thermal barriers that have limited Li–S battery practical deployment.
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Yiming Zhang, Yaoming Jiao, Guobing Tang, Qi Kang, Lianbo Ma (2026). Binary FeNi3 Alloy with Promoted Polysulfide Conversions Enabling Wide-Temperature Operation of High-Rate Lithium–Sulfur Batteries. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3946-2
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Frequently Asked Questions
What is the specific catalytic mechanism by which FeNi3 alloy enhances polysulfide conversion compared to pure Ni?
FeNi3 alloy exhibits a synergistic catalytic effect due to the electronic interaction between Fe and Ni atoms, which modulates the d-band center and enhances adsorption and conversion of polysulfides. Time-of-flight secondary ion mass spectroscopy and in situ XRD confirm a larger Li2S amount generated with FeNi3, indicating accelerated redox kinetics.
How does the FeNi3/CNS electrocatalyst perform under high sulfur loading and lean electrolyte conditions?
At a sulfur loading of ~4.0 mg cm−2, the FeNi3/CNS cathode achieves a maximum areal capacity of 5.60 mAh cm−2, demonstrating effective utilization of active material even at high loading. This suggests potential for practical high-energy-density cells, though lean electrolyte conditions were not explicitly tested in this study.
What is the long-term cycling stability of FeNi3/CNS-based Li-S batteries at high current rates?
The battery retains 639 mAh g−1 after 500 cycles at 1.0 C, corresponding to a capacity retention of approximately 75% (assuming initial capacity around 850 mAh g−1). This indicates robust cycling stability, which is critical for commercial applications.
How does the wide-temperature operation (−15 to 60°C) affect the electrochemical performance, and what are the underlying mechanisms?
The FeNi3/CNS catalyst maintains stable cycling and high specific capacities across the temperature range. At low temperatures, the alloy's catalytic activity mitigates sluggish kinetics due to increased electrolyte viscosity, while at high temperatures, it suppresses polysulfide shuttling, preventing rapid capacity loss. This dual functionality is attributed to the stable physicochemical properties of the alloy.
What are the potential scalability and cost implications of synthesizing FeNi3/CNS for industrial production?
The synthesis involves embedding FeNi3 nanoparticles in carbon nanosheets, which can be produced via scalable methods such as pyrolysis of metal precursors with carbon sources. Fe and Ni are abundant and low-cost, making the material economically viable. However, the uniformity of nanoparticle dispersion and reproducibility at scale remain challenges that need to be addressed.
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