article · Advanced Functional Materials
Lithium-sulfur batteries face practical limitations due to slow sulfur redox reaction kinetics and the shuttling of lithium polysulfides. To address these issues, a highly chaotic MXene-based heterostructure combining TiS2, TiN, TiO2, and Ti3C2Tx was synthesised using a straightforward solution-based method. The design demonstrates that increasing structural entropy enhances catalytic activity and suppresses polysulfide shuttling. Compared to a moderately chaotic counterpart and pristine MXene, this high-entropy material exhibits a lower Tafel slope and a higher electron transfer number. Density functional theory calculations indicate that introducing multiple phases lowers the energy barriers for key rate-limiting conversion and decomposition steps. When added at five weight percent to a sulfur cathode, the material significantly boosts the reversible capacity and rate capability of lithium-sulfur cells.
Lithium-sulfur batteries offer high theoretical energy storage, but their efficiency suffers from sluggish chemical reactions and internal material loss. By using a high-entropy design approach in catalyst materials, this research provides a clear method to accelerate battery reactions and stabilize chemistry, offering a clearer design principle for higher-performance energy storage technologies.
This research is at an early experimental stage, demonstrated through laboratory-scale cell testing. The primary application is high-energy lithium-sulfur batteries, potentially relevant to battery manufacturers and materials suppliers seeking to improve cathode performance. Because it requires only a small additive amount and uses a solution-based synthesis, the approach offers a possible route toward scalable cathode enhancement, though full-cell validation and manufacturing scale-up remain necessary.
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Abstract Both the sluggish sulfur redox reaction (SRR) kinetics and lithium polysulfides (LiPSs) shuttle effect limit the practical application of Li‐S batteries. Designing heterostructure sulfur hosts has emerged as an effective way to address these two issues with one material. However, the principles of heterostructures reinforced Li‐S batteries remain inadequately understood. Here, it is demonstrated for the first time that increasing the entropy of heterostructure can promote its SRR catalytic activity and alleviate the LiPSs shuttling. By a simple solution‐based strategy, a highly chaotic MXene‐based heterostructure (HCMH, TiS 2 /TiN/TiO 2 /Ti 3 C 2 T x ) is fabricated. The smart integration of “high entropy”, heterostructure, and MXene endow the HCMH catalyst with significantly improved performance, demonstrated by a much smaller Tafel slope of 62.9 mV dec −1 and a higher electron transfer number of 7.10, compared with the moderately chaotic MXene‐based heterostructure (MCMH, TiO 2 /TiN/Ti 3 C 2 T x ) and MXene. DFT theoretical calculations reveal that introducing new phases lowers the Gibbs energy barriers of both rate‐limiting Li 2 S 2 /Li 2 S reduction and Li 2 S decomposition. Upon the addition of only 5 wt.% HCMH to the sulfur cathode, both the reversible capacity and rate capability of Li‐S cells are greatly improved, which further highlights the importance of the high entropy “cocktail effect” in the design of SRR electrocatalysts in the future.
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DOI: 10.1002/adfm.202404976
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