A Designed High-Entropy Sulfide-Based Nanoporous Heterojunction for Fast, Durable, and High-Capacity Sodium Storage.

Ci, Naixuan; Yue, Xianke; Zhang, Yinghe; Cao, Boxuan; Ci, Lijie; Xie, Guoqiang; Liu, Xingjun; Reddy, Kolan Madhav et al. · Nano Lett · 2026

basic_science · Level V

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Abstract

As promising sodium ion battery (SIB) anodes, transition metal sulfide (TMS)-based heterojunctions still suffer from sluggish kinetics, low capacity, and structural instability. Herein, we design a nanoporous structured senary (AlCrCo)NiFeS<sub>2</sub>/MnS high-entropy heterojunction using dealloyed senary oxide as the starting materials. Owing to the high-entropy engineering-induced electronic structure regulation, the built-in electric field, the 3D nanoporous structure, and a hard carbon coating, the senary heterojunction exhibits a record high capacity of 885.5 mAh g<sup>-1</sup> after 110 cycles at 0.1 A g<sup>-1</sup>. Even at 40.0 A g<sup>-1</sup>, a high capacity of 331.5 mAh g<sup>-1</sup> can be achieved after 4000 cycles. DFT calculations reveal the modified electronic structure (denser energy band structure) induced by multiple-metal ion mixing, which enhances the electronic conductivity and sodium ion adsorption when compared with those of the ternary NiFeS<sub>2</sub>/MnS heterojunction. This work highlights the potential of high-entropy engineering for developing SIB anodes with one of the best overall performances.