Superstoichiometric reversible and manipulable copper-ion intercalation in niobium selenide

Yuanhe Sun, Rui Qi, Zhipeng Xue, Qi Lei, Yuanxin Zhao, Zhiguo Ren, Wei Zhang, Jingying Si, Haitao Li, Yi Gao, Wen Wen, Xiaolong Li () and Daming Zhu ()
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Yuanhe Sun: Chinese Academy of Sciences
Rui Qi: Chinese Academy of Sciences
Zhipeng Xue: Shanghai Jiaotong University
Qi Lei: Chinese Academy of Sciences
Yuanxin Zhao: Chinese Academy of Sciences
Zhiguo Ren: Chinese Academy of Sciences
Wei Zhang: Chinese Academy of Sciences
Jingying Si: Chinese Academy of Sciences
Haitao Li: Chinese Academy of Sciences
Yi Gao: Chinese Academy of Sciences
Wen Wen: Chinese Academy of Sciences
Xiaolong Li: Chinese Academy of Sciences
Daming Zhu: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Few-layer stacked niobium selenide (NbSe2) has evoked great interest owing to its intrinsically exotic properties and accessible manipulation by controlled ion intercalation for superconductivity physics and advanced device applications. However, attempts to extend the range of reversible intercalation stoichiometries are often hindered by overexpanded bond rupture and intrinsic-limit transition metal redox centres in selenides when proceeding towards deep intercalation. Here, we report that reversible unconventional superstoichiometric controlled intercalation in NbSe2 with up to two copper-ions per unit cell can be realized by triggering anionic redox, a fivefold improvement over previous report. Synergistic charge transfer of the transition metal and selenium framework inhibited the disorder of bonds and lattice structures to avoid falling into conversion, which is essential for obtaining superstoichiometric intercalation products, enabling tunable copper-ion de/intercalation repeatable for 11,000 cycles. Moreover, deep copper-ion intercalation and its derived intercalation compound family demonstrate milestone performance in capacity and cycling stability for extended electrochemical energy storage applications such as copper batteries, hybrid-ion zinc batteries, and nonaqueous potassium batteries. Our findings broaden the realm of intercalation compounds and offers appealing possibilities for tailoring on-demand physicochemical properties of materials towards the envisioned functional applications.

Date: 2025
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DOI: 10.1038/s41467-025-57423-3

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