Entropy-Stabilized Layered K 0.6 Ni 0.05 Fe 0.05 Mg 0.05 Ti 0.05 Mn 0.725 O 2 as a High-Rate and Stable Cathode for Potassium-Ion Batteries.
Yuqing CaiWenjing LiuFangfei ChangSu JinXusheng YangChuanxiang ZhangLing BaiTitus MaseseZiquan LiZhen-Dong HuangPublished in: ACS applied materials & interfaces (2023)
Mn-based layered oxides have been considered the most promising cathode candidates for cost-effective potassium-ion batteries (PIBs). Herein, equiatomic constituents of Ni, Fe, Mg, and Ti have been introduced into the transition metal layers of Mn-based layered oxide to design a high-entropy K 0.6 Ni 0.05 Fe 0.05 Mg 0.05 Ti 0.05 Mn 0.0725 O 2 (HE-KMO, S = 1.17R). Consequently, the experimental results manifest that the layered structure of HE-KMO is more stable than conventional low-entropy K 0.6 MnO 2 (LE-KMO, S = 0.66R) during successive cycling and even upon exposure to moisture. Diffraction and electrochemical measurements reveal that HE-KMO undergoes a solid-solution mechanism, contrary to the multistage phase transition processes typically exemplified in K 0.6 MnO 2 . Benefiting from the stabilized high-entropy layered framework and the solid-solution K + storage mechanism, the entropy-stabilized HE-KMO not only demonstrates exceptional rate capability but also shows excellent cyclic stability. Notably, a capacity retention ratio of 86% after 3000 cycles can still be sustained at a remarkable current density of 5000 mA g -1 .