Temperature Effects on Electrochemical Energy‐Storage Materials: A Case Study of Yttrium Niobate Porous Microspheres

Abstract Lithium‐ion batteries (LIBs) are very popular electrochemical energy‐storage devices. However, their applications in extreme environments are hindered because their low‐ and high‐temperature electrochemical performance is currently unsatisfactory. In order to build all‐climate LIBs, it is highly desirable to fully understand the underlying temperature effects on electrode materials. Here, based on a novel porous‐microspherical yttrium niobate (Y_0.5Nb_24.5O₆₂) model material, this work demonstrates that the operation temperature plays vital roles in electrolyte decomposition on electrode‐material surfaces, electrochemical kinetics, and crystal‐structure evolution. When the operation temperature increases, the reaction between the electrolyte and the electrode material become more intensive, causing the formation of thicker solid electrolyte interface (SEI) films, which decreases the initial Coulombic efficiency. Meanwhile, the electrochemical kinetics becomes faster, leading to the larger reversible capacity, higher rate capability, and more suitable working potential (i.e., lower working potential for anodes and higher working potential for cathodes). Additionally, the maximum unit‐cell‐volume change becomes larger, resulting in poorer cyclic stability. The insight gains here can provide a universal guide for the exploration of all‐climate electrode materials and their modification methods.