Self-Assembled Monolayer in Hybrid Quasi-Solid Electrolyte Enables Boosted Interface Stability and Ion Conduction.

Angew Chem Int Ed Engl

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620, China.

Published: November 2024

AI Article Synopsis

  • - The study investigates the challenges of interface stability in hybrid quasi-solid electrolytes (HQSE) due to complex interactions between inorganic solid electrolytes and liquid electrolytes, focusing on the ionic conductivity of the solid electrolyte's surface.
  • - A self-assembled monolayer using 4-chlorobenzenesulfonic acid (CBSA) is applied to the surface of LiLaZrTaO (LLZTO), resulting in improved interface stability and enhanced ionic conductivity and lithium transference in the HQSE.
  • - The enhanced performance of the modified HQSE is supported by experimental results showing no short-circuits after 1000 hours, with significant capacity retention in lithium iron phosphate (LFP) cells over

Article Abstract

Complex interactions between the inorganic solid electrolyte (ISE) and the liquid electrolyte (LE) give rise to challenges of achieving durable interface stability in hybrid quasi-solid electrolytes (HQSE), and the influence on the involved ISE surface ionic conductivity also needs to be investigated. Here, 4-chlorobenzenesulfonic acid (CBSA) is utilized to establish a self-assembled monolayer (SAM) on the surface of LiLaZrTaO (LLZTO), which is then incorporated into PEGDA-based in situ polymerized HQSE. The results show that the introduction of CBSA significantly improves the LLZTO/LE interface stability with the optimized solvation structure, resulting in a favorable ionic conductivity (1.19 mS⋅cm) and an increasing Li transference number (0.647). Mechanisms for the promotion of ionic conduction and interfacial stability of SAM-HQSE are unveiled through the density functional theory (DFT) combined with Raman spectra and Li solid-state nuclear-magnetic-resonance. There are no short-circuits in the Li|SAM-HQSE|Li cells after 1000 h. The LFP|SAM-HQSE|Li cells or LFP|SAM-HQSE|Graphite pouch cells respectively achieve the capacity retention of 91.2 % and 87.0 % with the 0.5.C-rate for 500 and 300 cycles. This facile and effective strategy proposed in this work make it accessible for constructing the stable surface micro-environments of LLZTO where boost and homogenize the Li conduction in a hybrid quasi-solid electrolyte system.

Download full-text PDF

Source
http://dx.doi.org/10.1002/anie.202418999DOI Listing

Publication Analysis

Top Keywords

hybrid quasi-solid
12
interface stability
12
self-assembled monolayer
8
quasi-solid electrolyte
8
ionic conductivity
8
monolayer hybrid
4
electrolyte
4
electrolyte enables
4
enables boosted
4
boosted interface
4

Similar Publications

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!