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Hierarchical SnS2@CNFs composite with 3D structure for high-performance aluminum-ion batteries: Unveiling Al3+ deintercalation mechanism through first-principles calculations

Journal 2025 · IF 6.3 · 发表于 2025 年 5 月 30 日
作者: Ruiyuan Zhuang,Yuxin Wang,Junhong Wang,Jianfeng Zhan,Jiangnan Yan,Yongqing Li,Yaru Chen,Wenhui Mo,Jian-chun Wu,Jianhong Yang,Lixiang Wang
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摘要

Aluminum ion batteries (AIBs) are deemed an encouraging prospect for energy storage applications owing to their beneficial attributes, including considerable theoretical specific capacity, heightened safety measures, affordability, and plentiful availability of materials. However, the inherent characteristics of cathode materials have greatly limited the further development of AIBs. In this work, SnS 2 @CNFs composites were prepared via a combination of hydrothermal and electrospinning strategy. Specifically, SnS 2 nanosheets, resembling flakes in their two-dimensional form, uniformly coated on the carbon fibers, forming a three-dimensional interconnected network seamlessly integrated with the continuous carbon substrate. This structure is conducive to shortening the ion transmission path, ensuring sufficient electrolyte contact, and facilitating electron transfer and transfer at the phase interfaces. As a self-supporting electrode for AIBs, the SnS 2 @CNFs electrode exhibited remarkable cyclability, retaining a residual capacity of approximately 70 mA h g −1 with a Coulombic efficiency close to 97 % after 500 cycles at 100 mA g −1 . The good cycle stability originates from the flexible carbon substrate effectively alleviating the volume expansion phenomenon caused by ion deintercalation in SnS 2 . In addition, first-principles calculations show that the substitution behavior of aluminum atoms in SnS 2 crystals exhibits obvious selectivity, but exceeding the energy threshold of conventional substitution reactions indicates that reactions are unlikely to occur. By constructing models to explore the embedding path of aluminum ions in SnS 2 crystals, the results showed that the embedding behavior mainly occurs in the van der Waals gap interstitial rather than within the crystal monolayer, and the sulfur atom top position is used as the optimal embedding site.

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