Order‐structured solid‐state electrolytes

Abstract

Solid-state electrolytes (SSEs) are recognized as attractive candidates to realize safe and high-energy-density lithium metal batteries (LMBs). However, the practical application of SSEs still faces challenges such as insufficient roomtemperature ionic conductivity, unsatisfactory mechanical properties, and large internal resistance. Extensive research efforts have been made to explore new electrochemistry and technologies to address those challenges. Among them, the construction of order-structured SSEs has emerged as a promising strategy.The anisotropic behavior induced by the orientation offers SSEs with desired properties targeting specific functions, and therefore the rational design of the order-structured SSE provides an alternative solution to achieve an ideal SSE. This review discusses the structure-property correlation of SSEs, and then summarizes the design strategies to construct order-structured SSEs. Finally, the current challenges and possible future research directions for order-structured SSEs for scalable high-energy-density LMBs are presented.

Designing mechanically reinforced filler network for thin and robust composite polymer electrolyte

“…In addition, the ordered filler structure can dissipate the mechanical impact energy through the interface and plastic deformation, thus enhancing the toughening effect. This facilitates further thickness reduction and inhibits dendrite growth to extend cell cycle life 25,67,113 …”

“…The 66 The improved ionic conductivity and mechanical properties of the resulting CPEs inhibit the growth of lithium dendrites and promote long-term cycling stability. 67 2.1 | Passive filler network with random structure…”

“…The electrolyte synthesized by Yang et al exhibits a perforation work level comparable to that of polypropylene separator membranes, thus showcasing superior dendrite resistance and long‐term cycle stability 66 . The improved ionic conductivity and mechanical properties of the resulting CPEs inhibit the growth of lithium dendrites and promote long‐term cycling stability 67 …”

Tailoring Vertically Aligned Inorganic‐Polymer Nanocomposites with Abundant Lewis Acid Sites for Ultra‐Stable Solid‐State Lithium Metal Batteries

“…[22][23][24][25][26][27][28][29] Among them, most fillers are randomly oriented in the polymer matrix with a high tortuosity, and the tortuous and discontinuous nature of the interface between polymer and fillers cannot maximize the ion transport capacity, where the orientation of these fillers has a great influence on the ionic conductivity. [30][31][32][33] Furthermore, some works demonstrate that when PSEs are stretched, the ionic conductivity in the vertical direction of the electrode is enhanced. Most strikingly, aligned fillers including montmorillonite, ceramic fibers, and aluminum oxide prepared by magnetic control, track-etching technique, and ice-templating method are highly desirable to guide ion transport and achieve high ionic conductivity.…”

“…Most strikingly, aligned fillers including montmorillonite, ceramic fibers, and aluminum oxide prepared by magnetic control, track-etching technique, and ice-templating method are highly desirable to guide ion transport and achieve high ionic conductivity. [30][31][32][33] As one of the most common hydrous minerals on Earth, akaganéite (β-FeOOH) exhibits a large tunnel-type monoclinic crystal structure framework with magnetic properties, and different structural designs such as nanorods will enrich its active sites by exposing reactive facets on the surface. [16] Some efforts have been devoted to controlling the size and shape of β-FeOOH to tailor unique properties and potential applications.…”