KLI

Reinforcing Native Solid-Electrolyte Interphase Layers via Electrolyte-Swellable Soft-Scaffold for Lithium Metal Anode

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Abstract
The lithium metal anode is notoriously unstable and reactive to electrolytes, forming brittle solid-electrolyte interphase (SEI) layers with uneven distribution, exacerbating Li dendrites that ultimately limit the battery life. Here, this work passivates Li metal with electrolyte-swellable polymer nanolayers deposited monolithically by the initiated chemical vapor deposition (iCVD) to reinforce the native SEI layers and stabilize their interface. The 100 nm iCVD poly(dimethylaminomethyl styrene) (pDMAMS) layer is swelled by 264% under a carbonate electrolyte, establishing the electrolyte-filled soft scaffold for Li-ion transport. Notably, the solvogel accommodates homogeneous Li2O-free and Li2CO3-rich native SEI layers, providing a record-high Li-ion transference number of 0.95 and ionic conductivity of 6.54 mS cm−1. The developed pDMAMS-Li anodes extend the cycle life by 550% in Li–Li symmetric cells and 600% in LiNi0.6Mn0.2Co0.2O2 full cells compared to pristine Li metal. The mechanistic details of the swollen-soft-scaffold strategy are elucidated by depth profile analysis of the pDMAMS homopolymer compared to pDMAMS/electrolyte-phobic copolymers, providing new insights to manage the interface of liquid-state electrolyte and solid-state Li metal by using a novel class of bifunctional solvogel.
Issued Date
2023
Jaehyeong Bae
Keonwoo Choi
Hyunsub Song
Do Heung Kim
Doo Young Youn
Su-Ho Cho
Dogyeong Jeon
Jiyoung Lee
Junyoung Lee
Wontae Jang
Changhyeon Lee
Youson Kim
Chanhoon Kim
Ji-Won Jung
Sung Gap Im
Il-Doo Kim
Type
Article
Keyword
electrolyte solvogelselectrolyte-swellable polymersinitiated CVDlithium dendriteslithium-metal battery anodessolid-electrolyte interphase layertransference number
DOI
10.1002/aenm.202203818
URI
https://oak.ulsan.ac.kr/handle/2021.oak/17472
Publisher
ADVANCED ENERGY MATERIALS
Language
영어
ISSN
1614-6832
Citation Volume
13
Citation Number
16
Citation Start Page
1
Citation End Page
12
Appears in Collections:
Engineering > Material Engineering
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