The metal sulfide or selenides have attracted increasing attention for high‐energy lithium‐ion batteries due to their unique layer structure flexibility, higher conductivity, and lower voltage polarization than metal oxides. However, low initial coulomb efficiency (ICE), serious structure destruction, and irreversible bonding chemistry are still big challenges for their practical application. Herein, layer GeSe₂ and its carbon composite are synthesized by high‐energy ball milling and it is surprisingly found that crystalline c‐GeSe₂ possesses higher reversible capacity and better rate performances than their amorphous counterparts. More specially, the broken GeSe bondings upon lithiation are also observed to regenerate after delithiation. These unusual phenomena are investigated by both experimental tools and theoretical calculations. Compared to other typical MX₂ (M = Mo, W, X = S, Se), the electronegativity of Ge is more close to selenium and the formation energy of GeSe bonding is much smaller. Thus, a mild driven force such as thermoheating at low temperature can recover the ordered layer structure, helping to heal the high conductivity and unimpeded Li diffusion pathways for crystalline GeSe₂. Similarly, electrochemical delithium force also triggers the rebuilding of GeSe bonding upon Li‐extraction, boosting GeSe₂/C with large capacity (1050 mA h g⁻¹), ultrahigh ICE (94%), and cycling stability.

中文翻译：

---

高性能锂离子电池层状GeSe2中热/电化学力触发的可修复结构

与金属氧化物相比，金属硫化物或硒化物具有独特的层结构柔韧性，更高的电导率和更低的电压极化，已引起高能锂离子电池越来越多的关注。然而，低的初始库仑效率（ICE），严重的结构破坏和不可逆的键合化学仍然是其实际应用的巨大挑战。本文中，GeSe ₂层及其碳复合物是通过高能球磨合成的，令人惊讶地发现，结晶c-GeSe _2的可逆容量和速率性能均优于非晶态对应物。更特别，破碎葛还观察到锂化时的硒键在脱锂后再生。通过实验工具和理论计算研究了这些异常现象。与其他典型的MX ₂（M = Mo，W，X = S，Se）相比，Ge的电负性更接近硒，GeSe键的形成能小得多。因此，适度的驱动力（例如在低温下加热）可以恢复有序的层结构，有助于修复高导电率和不受阻碍的晶体GeSe _2的Li扩散途径。类似地，电化学delithium力也触发Ge的重建在栗提取硒键合，增压GESE ₂ / C大容量（1050毫安汞柱^-1），超高ICE（94％）和循环稳定性。