Binary FeNi3 alloy with promoted polysulfide conversions enabling wide-temperature operation of high-rate lithium–sulfur batteries
摘要
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.