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

Abstract

Nanocomposite solid polymer electrolytes are considered as a promising strategy for solid‐state lithium metal batteries (SSLMBs). However, the randomly dispersed fillers in the polymer matrix with limited Li+ transference number and insufficient ionic conductivity severely sacrifice the ion transport capacity, thus restricting their practical application. To tackle these issues, a magnetic field‐assisted alignment strategy is proposed to disperse the vertically aligned akaganéite nanotube in the polymer matrix as an inorganic‐polymer nanocomposite solid‐state electrolyte for ultra‐stable SSLMBs. The metal cations as Lewis acid sites can grab anions to promote the dissociation of Li salts while the sufficient oxygen and hydroxyl functional group offer abundant Li‐ion migration sites for favored ion transportation. At the same time, the vertically aligned akaganéite/polymer interface combined with the above synergistic effects can establish oriented channels inside solid‐state electrolyte, which significantly elevates its ionic conductivity. Specially, an organic‐inorganic dual‐layer solid‐electrolyte interface is formed to uniform Li deposition and suppress the dendrite growth. The beneficial effect of the vertically aligned network is also demonstrated in full cell and pouch cell where remarkable 2000 cycles with a capacity decay of 0.012% per cycle can be achieved.

Practical challenges and future perspectives of solid polymer electrolytes: microscopic structure and interface design

“…The introduction of defect sites, such as oxygen vacancies, on inorganic fillers has been shown to regulate the local environment of Li + ions and decrease the activation energy for Li + ion transport. 128 Recently, Goodenough et al 129 investigated the local environments of Li + ions in SPEs. By introducing fillers with oxygen vacancies, which effectively enhanced the migration of Li + ions, they observed that the interactions between Li + ions and oxygen atoms in PEO were decreased compared to the interactions in the absence of fillers, proving that oxygen vacancies of fillers indeed can greatly enhance the migration of Li + ions.…”

“…The introduction of defect sites, such as oxygen vacancies, on inorganic fillers has been shown to regulate the local environment of Li + ions and decrease the activation energy for Li + ion transport. 128 Recently, Goodenough et al . 129 investigated the local environments of Li + ions in SPEs.…”

Balancing Charged Groups in Protein Additives: A Key to Enhancing the Performance of Polymer-Based Electrolytes in Solid-State Lithium–Metal Batteries

“…19,20 Wang et al 21 discovered that the incorporation of succinonitrile as a plasticizer effectively diminishes the crystallinity of PEO and can enable rapid Li + Following the above strategy, incorporating both positive and negative charge groups (CGs) into PEO-based SPEs to achieve the desired properties can also greatly enhance their ion conduction properties. For instance, Nie et al 22 utilized vertically aligned β-FeOOH fillers in the electrolyte. This configuration allows the anions to be captured by Fe 3+ ions, while the Li + transport was facilitated by the abundant hydroxyl groups on β-FeOOH's surface.…”

Coupling Anion‐Capturer with Polymer Chains in Fireproof Gel Polymer Electrolyte Enables Dendrite‐Free Sodium Metal Batteries

“…[20][21][22] In contrast, PEs based on polymer network have better mechanical flexibility, processability, and interfacial compatibility with electrode, and have distinctive advantages in the field of high-performance SSEs. [23,24] Among PEs, the ionic conductivity of gel polymer electrolytes (GPEs) can be comparable to liquid electrolytes, and the existence of the polymer network can effectively avoid the leakage of liquid components. [25,26] More importantly, the in situ constructed GPEs further enhance the interface compatibility, realizing the balance between safety, interface contact, and ionic conductivity.…”