Long-cycling and safe lithium metal batteries enabled by the synergetic strategy of <i>ex situ</i> anodic pretreatment and an in-built gel polymer electrolyte

et al. 2020

Angewandte Chemie

Zn batteries are usually considered as safe aqueous systems that are promising for flexible batteries. On the other hand, any liquids, including water, being encapsulated in a deformable battery may result in problems. Developing completely liquid‐free all‐solid‐state Zn batteries needs high‐quality solid‐state electrolytes (SSEs). Herein, we demonstrate in situ polymerized amorphous solid poly(1,3‐dioxolane) electrolytes, which show high Zn ion conductivity of 19.6 mS cm−1 at room temperature, low interfacial impedance, highly reversible Zn plating/stripping over 1800 h cycles, uniform and dendrite‐free Zn deposition, and non‐dry properties. The in‐plane interdigital‐structure device with the electrolyte completely exposed to the open atmosphere can be operated stably for over 30 days almost without weight loss or electrochemical performance decay. Furthermore, the sandwich‐structure device can normally operate over 40 min under exposure to fire. Meanwhile, the interfacial impedance and the capacity using in situ‐formed solid polymer electrolytes (SPEs) remain almost unchanged after various bending tests, a key criterion for flexible/wearable devices. Our study demonstrates an approach for SSEs that fulfill the requirement of no liquid and mechanical robustness for practical solid‐state Zn batteries.

Section: Resultsmentioning

confidence: 99%

Liquid‐Free All‐Solid‐State Zinc Batteries and Encapsulation‐Free Flexible Batteries Enabled by In Situ Constructed Polymer Electrolyte

et al. 2020

Angewandte Chemie

Section: Organoboron Based Additives For Pesmentioning

confidence: 99%

“…On one hand, Li et al selected LiDFOB as an initiator to start the in situ polymerization of poly-DOL GPE, forming integrated ionic connection between the electrode and the electrolyte. [116] On the other hand, by preprocessing the LMA and establishing a LiDFOB-LiTFSI dual-salt system, stable and compatible interfaces were successfully constructed in quasi-solid lithium metal batteries. The new poly-DOL GPE showed outstanding chemical compatibility with various intercalated cathodes (such as LiFePO 4 , LiMn 2 O 4, and LiCoO 2 ), and durable cycle life (Figure 10g).…”

Section: Borate Lithium Salts In Pes For In Situ Cationic Polymerizationmentioning

confidence: 99%

Organoboron‐Containing Polymer Electrolytes for High‐Performance Lithium Batteries

Dai

Zheng

Wei

2021

Adv Funct Materials

Polymer electrolytes (PEs) have been deemed as a sought‐after candidate for next‐generation lithium batteries. Substantial effort has been dedicated to exploiting PEs with improved comprehensive performance. Organoboron compounds have aroused great interest in PEs due to their distinct characteristics such as high design diversity, excellent thermal stability, promoting lithium‐ion transportation, and raising Li+ transference number. Organoboron compounds also have unique functions that facilitate the development of a stable solid electrolyte interface on the electrode surface. Their diversified structures and multiple functions are fundamentally associated with boron's hybridization form that determines the electronic structure of boron as a central atom. Here, recent advancement in organoboron‐containing PEs is reviewed in the aspect of polymer matrixes with boron moieties and organoboron additives for PEs. This review aims to highlight the diverse roles and high application potentials of organoboron compounds utilized in PEs. It is anticipated to provide a clear perspective of organoboron‐containing PEs and to spur more research interests for the exploration of safe and efficient lithium batteries.

“…[ 7–11 ] For achieving intimate interface contact and the compatibility with metallic lithium, an efficient and easy‐industrialized strategy is in situ solid poly‐ether electrolytes (SPEEs), which formed in electrochemical cells upgrading process by using conventional ether‐based electrolytes, like 1,3‐dioxolane (DOL) via cationic ring‐opening polymerization reaction. [ 3,12–15 ] However, it has two ineluctable problems including incomplete polymerization and residue of initiators, resulting in a “trade‐off” between ion conductivity and stability. Lewis‐acidic Li salts (e.g., LiPF 6 and LiDFOB) and organic metal compounds (e.g., Al(OTf) 3 and Sn(OTf) 4 ) are the two common initiators, which always trigger violent reactions.…”

Section: Introductionmentioning

confidence: 99%

In‐Built Quasi‐Solid‐State Poly‐Ether Electrolytes Enabling Stable Cycling of High‐Voltage and Wide‐Temperature Li Metal Batteries

Huo

et al. 2021

Adv Funct Materials

Developing solid‐state electrolytes with good compatibility for high‐voltage cathodes and reliable operation of batteries over a wide‐temperature‐range are two bottleneck requirements for practical applications of solid‐state metal batteries (SSMBs). Here, an in situ quasi solid‐state poly‐ether electrolyte (SPEE) with a nano‐hierarchical design is reported. A solid‐eutectic electrolyte is employed on the cathode surface to achieve highly‐stable performance in thermodynamic and electrochemical aspects. This performance is mainly due to an improved compatibility in the electrode/electrolyte interface by nano‐hierarchical SPEE and a reinforced interface stability, resulting in superb‐cyclic stability in Li||Li symmetric batteries (>4000 h at 1 mA cm−2/1 mAh cm−2; >2000 h at 1 mA cm−2/4 mAh cm−2), which are the same for Na, K, and Zn batteries. The SPEE enables outstanding cycle‐stability for wide‐temperature operation (15–100 °C) and 4 V‐above batteries (Li||LiCoO2 and Li||LiNi0.8Co0.1Mn0.1O2). The work paves the way for development of practical SSMBs that meet the demands for wide‐temperature applicability, high‐energy density, long lifespan, and mass production.