The lithium–sulfur (Li–S) battery is a promising candidate for next‐generation high‐density energy storage devices because of its ultrahigh theoretical energy density and the natural abundance of sulfur. However, the practical performance of the sulfur cathode is plagued by fast capacity decay and poor cycle life, both of which can be attributed to the intrinsic dissolution/shuttling of lithium polysulfides. Here, a new built‐in magnetic field–enhanced polysulfide trapping mechanism is discovered by introducing ferromagnetic iron/iron carbide (Fe/Fe3C) nanoparticles with a graphene shell (Fe/Fe3C/graphene) onto a flexible activated cotton textile (ACT) fiber to prepare the ACT@Fe/Fe3C/graphene sulfur host. The novel trapping mechanism is demonstrated by significant differences in the diffusion behavior of polysulfides in a custom‐designed liquid cell compared to a pure ACT/S cathode. Furthermore, a cell assembled using the ACT@Fe/Fe3C/S cathode exhibits a high initial discharge capacity of ≈764 mAh g−1, excellent rate performance, and a remarkably long lifespan of 600 cycles using ACT@Fe/Fe3C/S (whereas only 100 cycles can be achieved using pure ACT/S). The new magnetic field–enhanced trapping mechanism provides not only novel insight but unveils new possibilities for mitigating the “shuttle effect” of polysulfides thereby promoting the practical applications of Li–S batteries.
This content will become publicly available on December 1, 2024
Lithium dendrite‐induced short circuits and material loss are two major obstacles to the commercialization of lithium–sulfur (Li−S) batteries. Here, a nanocarbon composite consisting of cotton‐derived Fe3C‐encapsulated multiwalled carbon nanotubes (Fe3C‐MWCNTs) and graphene effectively traps polysulfides to suppress lithium dendrite growth is reported. Machine learning combined with molecular dynamics (MD) simulations unveils a new polysulfide‐induced lithium dendrite formation mechanism: the migration of polysulfides away from the anode drags out lithium protrusions through localized lattice distortion of the lithium anode and traps lithium ions in the surrounding electrolyte, leading to lithium dendrite formation. The Li−S battery, constructed using the composite of cotton‐derived Fe3C‐MWCNTs and graphene that serves as both the sulfur host and the anode interlayer, exhibits exceptional cycling stability, impressive capacity retention, and effective mitigation of lithium dendrite formation. The findings offer valuable strategies to prevent lithium dendrite formation and enhance understanding of lithium dendrite growth in Li−S batteries.
more » « less- NSF-PAR ID:
- 10478165
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Small
- ISSN:
- 1613-6810
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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