High-Entropy Prussian Blue Analogues as High-Capacity Cathode Material for Potassium Ion Batteries

Abstract

Potassium ion batteries, due to their similar electrochemical principles to lithium-ion batteries and the abundance of metal sources, are considered one of the alternatives to lithium-ion batteries. The development of new cathode materials has always been a research focus in this field. Among them, Prussian blue materials, with their three-dimensional open and flexible metal framework structure, can efficiently and reversibly store potassium ions. However, Prussian blue cathode materials still face issues such as poor reversibility and low capacity, which limit their application scope. This study investigates the preparation of high-entropy Prussian blue analogues materials to enhance electrochemical performance. The doping of five different transition metals (Fe2⁺, Co2⁺, Cu2+, Ni2+, and Mn2+) sharing the same nitrogen coordination sites results in a configurational entropy greater than 1.5 R for the material. HEPB-1 cathode material (K1.75Mn0.26Fe0.01Ni0.01Cu0.08Co0.09 [Fe(CN)6]0.66·0.83H2O) shows better electrochemical performance, with the initial discharge capacity of 86.69 and 74.51 mAh g−1 (capacity retention is 75.2% after 100 cycles) at 20 and 100 mA g−1, respectively. The research results have provided new insights for the further development and application of potassium ion batteries.