High-Capacity and Long-Life Aqueous Zn-SPAN Batteries with Tandem Catalysis.
basic_science · Level V
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- Record sourced from PubMed, PMID 39659126.
- Also identified by DOI 10.1002/adma.202409771.
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Abstract
Aqueous zinc-sulfur batteries are a high-capacity and cost-effective energy storage technology. However, the performance is plagued by the dissolution of intermediate polysulfides formed during conversion. Here, this issue is addressed by developing aqueous rechargeable Zn-sulfurized polyacrylonitrile (SPAN) batteries using tandem catalytic systems, containing water and tetraglyme (G4) with iodine (I<sub>2</sub>) additives. Mechanistic study and experiments reveal that the fully conjugated molecular configurations circumvent the formation of soluble polysulfides and enable reversible co-storage of H<sup>+</sup>/Zn<sup>2+</sup> with multiple redox-active centers. The reduced I<sub>2</sub> by G4 activates I<sup>-</sup>/I<sub>3</sub> <sup>-</sup> redox couple in SPAN, reducing activation energy, and accelerating Zn-ion transfer kinetics. Additionally, it stabilizes the Zn anode by forming an organic-inorganic interphase that induces the generation of the predominant (002) plane. The as-assembled Zn-SPAN batteries exhibit excellent performances, with a high capacity of 1260.4 mAh g<sup>-1</sup> at 0.2 A g<sup>-1</sup>, a high-rate performance (409.3 mAh g<sup>-1</sup> at 5 A g<sup>-1</sup>), and a long cycling stability (81.8% capacity remained over 800 cycles at 2 A g<sup>-1</sup>). This work takes a crucial step forward in organosulfur compounds accompanied by multi-electron transfer for the high-performance aqueous zinc-ion batteries.