Comonomer-Tuned Gel Electrolyte Enables Ultralong Cycle Life of Solid-State Lithium Metal Batteries

Fu, Yu1,2; Chen, Yifan1; Zhou, Limin1

2022-08-01

10.1021/acsami.2c09771

ACS Applied Materials & Interfaces   Impact Factor & Quartile

1944-8244

1944-8252

Rechargeable lithium metal batteries (LMBs) are considered the "holy grail " of energy storage systems. Unfortunately, uncontrollable dendritic lithium growth inherent in these batteries has prevented their practical applications. The benefits of solid-state electrolyte for LMBs are limited due to the common compromise between ionic conductivity and mechanical property. This work proposes a mechanism for simultaneous improvement in ionic conductivity and mechanical strength of gel polymer electrolyte (GPE) which is based on tunable cross-linked polymer network through adjusting monomer ratios. With increasing bisphenol A ethoxylate dimethacrylate (E2BADMA) and poly(ethylene glycol) diacrylate (PEGDA) mass ratios in GPE precursors, the formed polymer network experienced a composition evolution from a 3D cross-linked mono PEGDA network to triple PEGDA, E2BADMA, and PEGDA/E2BADMA networks and then to dual E2BADMA and PEGDA/E2BADMA networks, accompanied by the increase in both storage modulus (from 6 to 37 MPa) and ionic conductivity (from 0.06 to 0.44 mS cm-1). As a result, the E2BADMA/PEGDA mass ratio of 2:1 facilitates the successful fabrication of a dual-network-supported GPE (PEEPL-12) with a mechanical strength of 37 MPa and superior electrochemical properties (a high ionic conductivity of 0.44 mS cm-1 and a wide electrochemical stability window of 4.85 V vs Li/Li+). Such polymer electrolyte-based symmetric lithium metal batteries delivered a long cycle life (2000 h at 0.1 mA cm-2 and 0.1 mAh cm-2), and the Li|PEEPL-12|LiFePO4 cell delivered a high capacity of 140 mAh g-1 at the 100th cycle at the current density of 0.1 C (1 C = 170 mAh g-1). A more thorough investigation indicated the formation of a stable solid electrolyte interphase layer on a lithium metal anode. These extraordinary features open up a venue for fabrication of advanced polymer electrolyte for long-cycle-life lithium metal batteries.

cross-linked network lithium metal gel polymer electrolyte solid-state batteries solid electrolyte interface cycle life

SCI ; EI

English

First ; Corresponding

Southern University of Science and Technology, Tongji University[22120220149] ; Chinese Association of Science and Technology[2021QNRC001]

Science & Technology - Other Topics ; Materials Science

Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000854093200001

AMER CHEMICAL SOC

20223812752641

Charging (batteries) ; Crosslinking ; Interface states ; Ionic conduction in solids ; Ionic conductivity ; Ionic strength ; Iron compounds ; Lithium batteries ; Lithium compounds ; Metals ; Polyelectrolytes ; Polyethylene glycols ; Potentiometric sensors ; Solid electrolytes ; Solid state devices

Electricity: Basic Concepts and Phenomena:701.1 ; Primary Batteries:702.1.1 ; Secondary Batteries:702.1.2 ; Semiconductor Devices and Integrated Circuits:714.2 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Organic Polymers:815.1.1 ; Polymer Products:817.1 ; Classical Physics; Quantum Theory; Relativity:931 ; High Energy Physics; Nuclear Physics; Plasma Physics:932

Web of Science

1.Southern Univ Sci & Technol, Sch Syst Design & Intelligent Mfg, Shenzhen 518055, Guangdong, Peoples R China
2.Tongji Univ, Sch Aerosp Engn & Appl Mech, Shanghai 200092, Peoples R China

Fu, Yu,Chen, Yifan,Zhou, Limin. Comonomer-Tuned Gel Electrolyte Enables Ultralong Cycle Life of Solid-State Lithium Metal Batteries[J]. ACS Applied Materials & Interfaces,2022,14(36).

Fu, Yu,Chen, Yifan,&Zhou, Limin.(2022).Comonomer-Tuned Gel Electrolyte Enables Ultralong Cycle Life of Solid-State Lithium Metal Batteries.ACS Applied Materials & Interfaces,14(36).

Fu, Yu,et al."Comonomer-Tuned Gel Electrolyte Enables Ultralong Cycle Life of Solid-State Lithium Metal Batteries".ACS Applied Materials & Interfaces 14.36(2022).